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Abstract:

Non-cementitious CO2 sequestering compositions are provided. The
compositions of the invention include a CO2 sequestering additive,
e.g., a CO2 sequestering carbonate composition. Additional aspects
of the invention include methods of making and using the non-cementitious
CO2 sequestering compositions.

Claims:

1-2. (canceled)

3. A method of forming a non-cementitious composition, comprising:
precipitating a CO2 sequestering composition by contacting CO2
released from combustion of fuel with an aqueous composition, wherein
said CO2 sequestering composition comprises carbon from said
CO2; and producing a non-cementitious composition comprising said
CO2 sequestering composition in an amount of 1% by weight or more.

4. The method of claim 3, wherein said precipitating comprises removing
protons from said aqueous composition using a proton-removing agent.

12. The method of claim 11, wherein said environmental remediation
product is forest soil restoration or neutralization of over-acidified
water.

13. The method of claim 3, wherein said CO2 sequestering composition
is in said amount of 5-75% w/w in said non-cementitious composition.

14. The method of claim 3, wherein said CO2 sequestering composition
is in a storage stable form.

15. The method of claim 3, wherein said fuel is fossil fuel.

16. The method of claim 3, wherein said CO2 sequestering composition
stores 50 tons or more of said CO.sub.2.

17. The method of claim 3, wherein said CO2 sequestering composition
comprises 5% or more of said CO2 as carbonate compound.

18. The method of claim 17, wherein said carbonate compound is a
metastable carbonate compound selected from the group consisting of
vaterite, aragonite, amorphous calcium carbonate, and combination
thereof.

[0002] Carbon dioxide (CO2) emissions have been identified as a major
contributor to the phenomenon of global warming and ocean acidification.
CO2 is a by-product of combustion and it creates operational,
economic, and environmental problems. It is expected that elevated
atmospheric concentrations of CO2 and other greenhouse gases will
facilitate greater storage of heat within the atmosphere leading to
enhanced surface temperatures and rapid climate change. CO2 has also
been interacting with the oceans driving down the pH toward 8.0. CO2
monitoring has shown atmospheric CO2 has risen from approximately
280 ppm in the 1950s to approximately 380 pmm today, and is expect to
exceed 400 ppm in the next decade. The impact of climate change will
likely be economically expensive and environmentally hazardous. Reducing
potential risks of climate change will require sequestration of
atmospheric CO2.

SUMMARY OF THE INVENTION

[0003] In some embodiments, the invention provides a non-cementitious
composition that includes a CO2 sequestering additive, in which the
CO2 sequestering additive includes carbon that was released in the
form of CO2 from the combustion of fuel. In some embodiments, the
invention provides a non-cementitious composition in which the CO2
sequestering additive is a carbonate compound. In some embodiments, the
invention provides a non-cementitious composition in which the carbonate
compound composition includes a precipitate from an
alkaline-earth-metal-containing water. In some embodiments, the invention
provides a non-cementitious composition in which the
alkaline-earth-metal-containing water from which the carbonate compound
composition precipitate forms includes CO2 derived from an
industrial waste stream. In some embodiments, the invention provides a
non-cementitious composition in which the non-cementitious composition is
a paper product. In some embodiments, the invention provides a
non-cementitious composition in which the non-cementitious composition is
a polymeric product. In some embodiments, the invention provides a
non-cementitious composition in which the non-cementitious composition is
a lubricant. In some embodiments, the invention provides a
non-cementitious composition in which the non-cementitious composition is
an adhesive. In some embodiments, the invention provides a
non-cementitious composition in which the non-cementitious composition is
rubber. In some embodiments, the invention provides a non-cementitious
composition in which the non-cementitious composition is chalk. In some
embodiments, the invention provides a non-cementitious composition in
which the non-cementitious composition is an asphalt product. In some
embodiments, the invention provides a non-cementitious composition in
which the non-cementitious composition is paint. In some embodiments, the
invention provides a non-cementitious composition in which the
non-cementitious composition is an abrasive for paint removal. In some
embodiments, the invention provides a non-cementitious composition in
which the non-cementitious composition is a personal care product. In
some embodiments, the invention provides a non-cementitious composition
that is a personal care product in which the personal care product is a
cosmetic. In some embodiments, the invention provides a non-cementitious
composition that is a personal care product in which the personal care
product is a cleaning product. In some embodiments, the invention
provides a non-cementitious composition that is a personal care product
in which the personal care product is a personal hygiene product. In some
embodiments, the invention provides a non-cementitious composition in
which the non-cementitious composition is an ingestible product. In some
embodiments, the invention provides a non-cementitious composition that
is an ingestible product, in which the ingestible product is a liquid. In
some embodiments, the invention provides a non-cementitious composition
that is an ingestible product, in which the ingestible product is a
solid. In some embodiments, the invention provides a non-cementitious
composition that is an ingestible product, in which the ingestible
product is an animal ingestible product. In some embodiments, the
invention provides a non-cementitious composition in which the
non-cementitious composition is an agricultural product. In some
embodiments, the invention provides a non-cementitious composition that
is an agricultural product, in which the agricultural product is a soil
amendment product. In some embodiments, the invention provides a
non-cementitious composition that is an agricultural product, in which
the agricultural product is a pesticide. In some embodiments, the
invention provides a non-cementitious composition in which the
non-cementitious composition is an environmental remediation product. In
some embodiments, the invention provides a non-cementitious composition
that is an environmental remediation product in which the environmental
remediation product is forest soil restoration. In some embodiments, the
invention provides a non-cementitious composition that is an
environmental remediation product in which the environmental remediation
product is neutralization of over-acidified water.

[0004] In some embodiments, the invention provides a method of producing a
non-cementitious composition, in which the method includes obtaining a
CO2 sequestering additive, in which the CO2 sequestering
additive includes carbon that was released in the form of CO2 from
the combustion of fuel and producing a non-cementitious composition that
includes the CO2 sequestering additive. In some embodiments, the
invention provides a method of producing a non-cementitious composition
in which the CO2 sequestering additive is a carbonate compound
composition. In some embodiments, the invention provides a method of
producing a non-cementitious composition in which the carbonate compound
composition includes a precipitate from an
alkaline-earth-metal-containing water. In some embodiments, the invention
provides a method of producing a non-cementitious composition in which
the alkaline-earth-metal-containing water includes CO2 derived from
an industrial waste stream. In some embodiments, the invention provides a
method of producing a non-cementitious composition in which the
non-cementitious composition is a paper product. In some embodiments, the
invention provides a method of producing a non-cementitious composition
in which the non-cementitious composition is a lubricant. In some
embodiments, the invention provides a method of producing a
non-cementitious composition in which the non-cementitious composition is
an adhesive. In some embodiments, the invention provides a method of
producing a non-cementitious composition in which the non-cementitious
composition is rubber. In some embodiments, the invention provides a
method of producing a non-cementitious composition in which the
non-cementitious composition is chalk. In some embodiments, the invention
provides a method of producing a non-cementitious composition in which
the non-cementitious composition is an asphalt product. In some
embodiments, the invention provides a method of producing a
non-cementitious composition in which the non-cementitious composition is
paint. In some embodiments, the invention provides a method of producing
a non-cementitious composition in which the non-cementitious composition
is an abrasive for paint removal. In some embodiments, the invention
provides a method of producing a non-cementitious composition in which
the non-cementitious composition is a personal care product. In some
embodiments, the invention provides a method of producing a
non-cementitious composition that is a personal care product, in which
the personal care product is a cosmetic. In some embodiments, the
invention provides a method of producing a non-cementitious composition
that is a personal care product, in which the personal care product is a
cleaning product. In some embodiments, the invention provides a method of
producing a non-cementitious composition that is a personal care product,
in which the personal care product is a personal hygiene product. In some
embodiments, the invention provides a method of producing a
non-cementitious composition in which the non-cementitious composition is
an ingestible product. In some embodiments, the invention provides a
method of producing a non-cementitious composition that is an ingestible
product, in which the ingestible product is a liquid. In some
embodiments, the invention provides a method of producing a
non-cementitious composition that is an ingestible product, in which the
ingestible product is a solid. In some embodiments, the invention
provides a method of producing a non-cementitious composition in which
the non-cementitious composition is an animal ingestible product. In some
embodiments, the invention provides a method of producing a
non-cementitious composition in which the non-cementitious composition is
an agricultural product. In some embodiments, the invention provides a
method of producing a non-cementitious composition that is an
agricultural product, in which the agricultural product is a soil
amendment product. In some embodiments, the invention provides a method
of producing a non-cementitious composition that is an agricultural
product, in which the agricultural product is a pesticide. In some
embodiments, the invention provides a method of producing a
non-cementitious composition in which the non-cementitious composition is
an environmental remediation product. In some embodiments, the invention
provides a method of producing a non-cementitious that is an
environmental remediation product, in which environmental remediation
product is forest soil restoration. In some embodiments, the invention
provides a method of producing a non-cementitious that is an
environmental remediation product, in which environmental remediation
product is neutralization of over-acidified water.

[0005] In some embodiments, the invention provides a method of
sequestering carbon dioxide that includes precipitating a CO2
sequestering carbonate compound composition from an
alkaline-earth-metal-containing water, in which the carbonate compound
composition includes carbon that was released in the form of CO2
from the combustion of fuel and producing a CO2 sequestering
additive comprising the carbonate compound composition and producing a
non-cementitious composition comprising the CO2 sequestering
additive. In some embodiments, the invention provides a method of
sequestering carbon dioxide in which the alkaline-earth-metal-containing
water is contacted to an industrial waste stream prior to the
precipitation step.

INCORPORATION BY REFERENCE

[0006] All publications, patents, and patent applications mentioned in
this specification are herein incorporated by reference to the same
extent as if each individual publication, patent, or patent application
was specifically and individually indicated to be incorporated by
reference.

BRIEF DESCRIPTION OF THE DRAWINGS

[0007] The novel features of the invention are set forth with
particularity in the appended claims. A better understanding of the
features and advantages of the present invention will be obtained by
reference to the following detailed description that sets forth
illustrative embodiments, in which the principles of the invention are
utilized, and the accompanying drawings of which:

[0008] FIG. 1 provides a schematic of a CO2 sequestering additive
production process according to an embodiment of the invention.

DETAILED DESCRIPTION OF THE INVENTION

[0009] Non-cementitious CO2 sequestering compositions are provided.
The compositions of the invention include a CO2 sequestering
additive, e.g., a CO2 sequestering carbonate composition. Additional
aspects of the invention include methods of making and using the
non-cementitious CO2 sequestering compositions.

[0010] Before the present invention is described in greater detail, it is
to be understood that this invention is not limited to particular
embodiments described, as such may, of course, vary. It is also to be
understood that the terminology used herein is for the purpose of
describing particular embodiments only, and is not intended to be
limiting, since the scope of the present invention will be limited only
by the appended claims.

[0011] Where a range of values is provided, it is understood that each
intervening value, to the tenth of the unit of the lower limit unless the
context clearly dictates otherwise, between the upper and lower limit of
that range and any other stated or intervening value in that stated
range, is encompassed within the invention. The upper and lower limits of
these smaller ranges may independently be included in the smaller ranges
and are also encompassed within the invention, subject to any
specifically excluded limit in the stated range. Where the stated range
includes one or both of the limits, ranges excluding either or both of
those included limits are also included in the invention.

[0012] Certain ranges are presented herein with numerical values being
preceded by the term "about." The term "about" is used herein to provide
literal support for the exact number that it precedes, as well as a
number that is near to or approximately the number that the term
precedes. In determining whether a number is near to or approximately a
specifically recited number, the near or approximating unrecited number
may be a number which, in the context in which it is presented, provides
the substantial equivalent of the specifically recited number.

[0013] Unless defined otherwise, all technical and scientific terms used
herein have the same meaning as commonly understood by one of ordinary
skill in the art to which this invention belongs. Although any methods
and materials similar or equivalent to those described herein can also be
used in the practice or testing of the present invention, representative
illustrative methods and materials are now described.

[0014] All publications and patents cited in this specification are herein
incorporated by reference as if each individual publication or patent
were specifically and individually indicated to be incorporated by
reference and are incorporated herein by reference to disclose and
describe the methods and/or materials in connection with which the
publications are cited. The citation of any publication is for its
disclosure prior to the filing date and should not be construed as an
admission that the present invention is not entitled to antedate such
publication by virtue of prior invention. Further, the dates of
publication provided may be different from the actual publication dates
which may need to be independently confirmed.

[0015] It is noted that, as used herein and in the appended claims, the
singular forms "a," "an," and "the" include plural references unless the
context clearly dictates otherwise. It is further noted that the claims
may be drafted to exclude any optional element. As such, this statement
is intended to serve as antecedent basis for use of such exclusive
terminology as "solely," "only" and the like in connection with the
recitation of claim elements, or use of a "negative" limitation.

[0016] As will be apparent to those of skill in the art upon reading this
disclosure, each of the individual embodiments described and illustrated
herein has discrete components and features which may be readily
separated from or combined with the features of any of the other several
embodiments without departing from the scope or spirit of the present
invention. Any recited method can be carried out in the order of events
recited or in any other order which is logically possible.

[0017] In further describing the subject invention, embodiments of the
non-cementitious CO2 sequestering compositions, as well as methods
and systems for their production, will be described first in greater
detail. Next, examples of methods of using the CO2 sequestering
compositions will be reviewed further.

Non-Cementitious CO2 Sequestering Compositions

[0018] Non-cementitious CO2 sequestering compositions are provided by
the invention. By "CO2 sequestering composition" is meant that the
composition contains carbon derived from a fuel used by humans, e.g.,
carbon having a fossil fuel origin. For example, CO2 sequestering
compositions according to aspects of the present invention contain carbon
that was released in the form of CO2 from the combustion of fuel. In
certain embodiments, the carbon sequestered in a CO2 sequestering
composition is in the form of a carbonate compound. Therefore, in certain
embodiments, CO2 sequestering compositions according to aspects of
the subject invention contain carbonate compounds where at least part of
the carbon in the carbonate compounds is derived from a fuel used by
humans, e.g., a fossil fuel. As such, production of compositions of the
invention results in the placement of CO2 into a storage stable
form, e.g., a stable component of a non-cementitious composition.
Production of the CO2 sequestering compositions of the invention
thus results in the prevention of CO2 gas from entering the
atmosphere. The compositions of the invention provide for storage of
CO2 in a manner such that CO2 sequestered (i.e., fixed) in the
composition does not become part of the atmosphere. Compositions of the
invention keep their sequestered CO2 fixed for substantially the
useful life the composition, if not longer, without significant, if any,
release of the CO2 from the composition. As such, where the
compositions are consumable compositions, the CO2 fixed therein
remains fixed for the life of the consumable, if not longer.

[0019] CO2 sequestering compositions of the invention include
compositions that contain carbonates and/or bicarbonates, which may be in
combination with a divalent cation such as calcium and/or magnesium, or
with a monovalent cation such as sodium. The carbonates and/or
bicarbonates may be in solution, in solid form, or a combination of
solution and solid form, e.g., a slurry. The carbonates and/or
bicarbonates may contain carbon dioxide from a source of carbon dioxide;
in some embodiments the carbon dioxide originates from the burning of
fossil fuel, and thus some (e.g., at least 10, 50, 60, 70, 80, 90, 95%)
or substantially all (e.g., at least 99, 99.5, or 99.9%) of the carbon in
the carbonates and/or bicarbonates is of fossil fuel origin, i.e., of
plant origin. As is known, carbon of plant origin has a different ratio
of stable isotopes (13C and 12C) than carbon of inorganic
origin, and thus the carbon in the carbonates and/or bicarbonates, in
some embodiments, has a δ13C of less than, e.g.,
-10.Salinity., or less than -15.Salinity., or less than -20.Salinity., or
less than -35.Salinity., or less than -30.Salinity., or less than
-35.Salinity. as described in further detail herein below.

[0020] Compositions of the invention include a CO2 sequestering
additive. CO2 sequestering additives are components that store a
significant amount of CO2 in a storage stable format, such that
CO2 gas is not readily produced from the product and released into
the atmosphere. In certain embodiments, the CO2 sequestering
additives can store 50 tons or more of CO2, such as 100 tons or more
of CO2, including 250 tons or more of CO2, for instance 500
tons or more of CO2, such as 750 tons or more of CO2, including
900 tons or more of CO2 for every 1000 tons of composition of the
invention. In certain embodiments, the CO2 sequestering additives of
the compositions of the invention comprise about 5% or more of CO2,
such as about 10% or more of CO2, including about 25% or more of
CO2, for instance about 50% or more of CO2, such as about 75%
or more of CO2, including about 90% or more of CO2, e.g.,
present as one or more carbonate compounds.

[0021] The CO2 sequestering additives of the invention may include
one or more carbonate compounds. The amount of carbonate in the CO2
sequestering additive, as determined by coulometry using the protocol
described in coulometric titration, may be 40% or higher, such as 70% or
higher, including 80% or higher. In some embodiments, where the Mg source
is a mafic mineral (as described in U.S. Provisional Application Ser. No.
61/079,790, incorporated by reference herein), or an ash (as described in
U.S. Provisional Application Ser. No. 61/073,319, incorporated herein by
reference), the resultant product may be a composition containing silica
as well as carbonate. In these embodiments, the carbonate content of the
product may be as low as 10%.

[0022] The carbonate compounds of the CO2 sequestering additives may
be metastable carbonate compounds that are precipitated from a water,
such as a salt-water, as described in greater detail below. The carbonate
compound compositions of the invention include precipitated crystalline
and/or amorphous carbonate compounds. Specific carbonate minerals of
interest include, but are not limited to: calcium carbonate minerals,
magnesium carbonate minerals and calcium magnesium carbonate minerals.
Calcium carbonate minerals of interest include, but are not limited to:
calcite (CaCO3), aragonite (CaCO3), vaterite (CaCO3),
ikaite (CaCO3.6H2O), and amorphous calcium
carbonate(CaCO3.nH2O). Magnesium carbonate minerals of interest
include, but are not limited to: magnesite (MgCO3), barringtonite
(MgCO3.2H2O), nesquehonite (MgCO3.3H2O), lanfordite
(MgCO3.5H2O) and amorphous magnesium calcium carbonate
(MgCO3.nH2O). Calcium magnesium carbonate minerals of interest
include, but are not limited to dolomite (CaMgCO3), huntite
(CaMg3(CO3)4) and sergeevite
(Ca2Mg11(CO3)13H2O). In certain embodiments,
non-carbonate compounds like brucite (Mg(OH)2) may also form in
combination with the minerals listed above. As indicated above, the
compounds of the carbonate compound compositions are metastable carbonate
compounds (and may include one or more metastable hydroxide compounds)
that are more stable in saltwater than in freshwater, such that upon
contact with fresh water of any pH they dissolve and re-precipitate into
other fresh water stable compounds, e.g., minerals such as low-Mg
calcite.

[0023] The CO2 sequestering additives of the invention are derived
from, e.g., precipitated from, a water (as described in greater detail
below). As the CO2 sequestering products are precipitated from a
water, they may include one or more additives that are present in the
water from which they are derived. For example, where the water is salt
water, the CO2 sequestering products may include one or more
compounds found in the salt water source. These compounds may be used to
identify the solid precipitations of the compositions that come from the
salt water source, where these identifying components and the amounts
thereof are collectively referred to herein as a saltwater source
identifier. For example, if the saltwater source is sea water,
identifying compounds that may be present in the precipitated solids of
the compositions include, but are not limited to: chloride, sodium,
sulfur, potassium, bromide, silicon, strontium and the like. Any such
source-identifying or "marker" elements would generally be present in
small amounts, e.g., in amounts of 20,000 ppm or less, such as amounts of
2000 ppm or less. In certain embodiments, the "marker" compound is
strontium, which may be present in the precipitated incorporated into the
aragonite lattice, and make up 10,000 ppm or less, ranging in certain
embodiments from 3 to 10,000 ppm, such as from 5 to 5000 ppm, including 5
to 1000 ppm, e.g., 5 to 500 ppm, including 5 to 100 ppm. Another "marker"
compound of interest is magnesium, which may be present in amounts of up
to 20% mole substitution for calcium in carbonate compounds. The
saltwater source identifier of the compositions may vary depending on the
particular saltwater source employed to produce the saltwater-derived
carbonate composition. Also of interest are isotopic markers that
identify the water source.

[0024] Depending on the particular non-cementitious material or product,
the amount of CO2 sequestering additive that is present may vary. In
some instances, the amount of CO2 sequestering additive ranges from
5 to 75% w/w, such as 5 to 50% w/w including 5 to 25% w/w and including 5
to 10% w/w.

[0025] The compositions of the invention may be viewed as low-carbon
footprint compositions. Low-carbon footprint compositions have a reduced
carbon footprint as compared to corresponding compositions that lack the
CO2 sequestering additive (where "corresponding" herein means the
identical composition but for the presence of the CO2 sequestering
additive of the invention). Using any convenient carbon footprint
calculator, the magnitude of carbon footprint reduction of the
compositions of the invention as compared to corresponding compositions
that lack the CO2 sequestering additive may be 5% or more, such as
10% or more, including 25%, 50%, 75% or even 100% or more. In certain
embodiments, the low-carbon footprint compositions of the invention are
carbon neutral, in that they have substantially no, if any, calculated
carbon footprint, e.g., as determined using any convenient carbon
footprint calculator that is relevant for a particular composition of
interest. Carbon neutral compositions of the invention include those
compositions that exhibit a carbon footprint of 50 lbs CO2/cu yd
material or less, such as 10 lbs CO2/cu yd material or less,
including 5 lbs CO2/cu yd material or less, where in certain
embodiments the carbon neutral compositions have 0 or negative lbs
CO2/cu yd material, such as negative 1 or more, e.g., negative 3 or
more lbs CO2/cu yd material. In some instances, the low carbon
footprint compositions have a significantly negative carbon footprint,
e.g., -100 or more lbs CO2/cu yd or less.

[0026] In certain embodiments compositions of the invention will contain
carbon from fossil fuel; because of its fossil fuel origin, the carbon
isotopic fractionation (δ13C) value of such compositions will
be different from that of compositions containing inorganic carbon, e.g.,
limestone. As is known in the art, the plants from which fossil fuels are
derived preferentially utilize 12C over 13C, thus fractionating
the carbon isotopes so that the value of their ratio differs from that in
the atmosphere in general; this value, when compared to a standard value
(PeeDee Belemnite, or PDB, standard), is termed the carbon isotopic
fractionation (δ13C) value. δ13C values for coal
are generally in the range -30 to -20.Salinity. and δ13C
values for methane may be as low as -20.Salinity. to -40.Salinity. or
even -40.Salinity. to -80.Salinity.. δ13C values for
atmospheric CO2 are -10.Salinity. to -7.Salinity., for limestone
+3.Salinity. to -3.Salinity., and for marine bicarbonate, 0.Salinity..
Even if the non-cementitious material contains some natural limestone, or
other source of C with a higher (less negative) δ13C value
than fossil fuel, its δ13C value generally will still be
negative and less than (more negative than) values for limestone or
atmospheric CO2. In some embodiments, the non-cementitious material
or product includes a CO2-sequestering additive comprising
carbonates, bicarbonates, or a combination thereof, in which the
carbonates, bicarbonates, or a combination thereof have a carbon isotopic
fractionation (δ13C) value less than -5.00.Salinity..
Compositions of the invention thus includes a non-cementitious material
or product with a δ13C less than -10.Salinity., such as less
than -12.Salinity., -14.Salinity., -16.Salinity., -18.Salinity.,
-20.Salinity., -22.Salinity., -24.Salinity., -26.Salinity.,
-28.Salinity., or less than -30.Salinity.. In some embodiments the
invention provides a non-cementitious material or product with a
δ13C less than -10.Salinity.. In some embodiments the
invention provides a non-cementitious material or product with a
δ13C less than -14.Salinity.. In some embodiments the
invention provides a non-cementitious material or product with a
δ13C less than -18.Salinity.. In some embodiments the
invention provides a non-cementitious material or product with a
δ13C less than -20.Salinity.. In some embodiments the
invention provides a non-cementitious material or product with a
δ13C less than -24.Salinity.. In some embodiments the
invention provides a non-cementitious material or product with a
δ13C less than -28.Salinity.. In some embodiments the
invention provides a non-cementitious material or product with a
δ13C less than -30.Salinity.. In some embodiments the
invention provides a non-cementitious material or product with a
δ13C less than -32.Salinity.. In some embodiments the
invention provides a non-cementitious material or product with a
δ13C less than -34.Salinity.. Such a non-cementitious
materials or products may be carbonate-containing materials or products,
as described above, e.g., a non-cementitious material or product with
that contains at least 10, 20, 30, 40, 50, 60, 70, 80, or 90% carbonate,
e.g., at least 50% carbonate w/w.

[0027] The relative carbon isotope composition (δ13C) value
with units of .Salinity. (per mil) is a measure of the ratio of the
concentration of two stable isotopes of carbon, namely 12C and
13C, relative to a standard of fossilized belemnite (the PDB
standard).

[0028]12C is preferentially taken up by plants during photosynthesis
and in other biological processes that use inorganic carbon because of
its lower mass. The lower mass of 12C allows for kinetically limited
reactions to proceed more efficiently than with 13C. Thus, materials
that are derived from plant material, e.g., fossil fuels, have relative
carbon isotope composition values that are less than those derived from
inorganic sources. The carbon dioxide in flue gas produced from burning
fossil fuels reflects the relative carbon isotope composition values of
the organic material that was fossilized. Table 1 lists relative carbon
isotope composition value ranges for relevant carbon sources for
comparison.

[0029] Material incorporating carbon from burning fossil fuels reflects
δ13C values that are more like those of plant derived
material, i.e. less, than that which incorporates carbon from atmospheric
or non-plant marine sources. Verification that the material produced by a
carbon dioxide sequestering process is composed of carbon from burning
fossil fuels can include measuring the δ13C value of the
resultant material and confirming that it is not similar to the values
for atmospheric carbon dioxide, nor marine sources of carbon.

[0030] In some embodiments the invention provides a method of
characterizing a composition comprising measuring its relative carbon
isotope composition (δ13C) value. In some embodiments the
composition is a composition that contains carbonates, e.g., magnesium
and/or calcium carbonates. Any suitable method may be used for measuring
the δ13C value, such as mass spectrometry or off-axis
integrated-cavity output spectroscopy (off-axis ICOS).

[0031] One difference between the carbon isotopes is in their mass. Any
mass-discerning technique sensitive enough to measure the amounts of
carbon we have can be used to find ratios of the 13C to 12C
isotope concentrations. Mass spectrometry is commonly used to find
δ13C values. Commercially available are bench-top off-axis
integrated-cavity output spectroscopy (off-axis ICOS) instruments that
are able to determine δ13C values as well. These values are
obtained by the differences in the energies in the carbon-oxygen double
bonds made by the 12C and 13C isotopes in carbon dioxide. The
δ13C value of a carbonate precipitate from a carbon
sequestration process serves as a fingerprint for a CO2 gas source,
as the value will vary from source to source, but in most carbon
sequestration cases δ13C will generally be in a range of
-9.Salinity. to -35.Salinity..

[0032] In some embodiments the methods further include the measurement of
the amount of carbon in the composition. Any suitable technique for the
measurement of carbon may be used, such as coulometry.

[0033] Precipitation material, which comprises one or more synthetic
carbonates derived from industrial CO2, reflects the relative carbon
isotope composition (δ13C) of the fossil fuel (e.g., coal,
oil, natural gas, or flue gas) from which the industrial CO2 (from
combustion of the fossil fuel) was derived. The relative carbon isotope
composition (δ13C) value with units of .Salinity. (per mille)
is a measure of the ratio of the concentration of two stable isotopes of
carbon, namely 12C and 13C, relative to a standard of
fossilized belemnite (the PDB standard).

[0034] As such, the δ13C value of the CO2 sequestering
additive serves as a fingerprint for a CO2 gas source. The
δ13C value may vary from source to source (i.e., fossil fuel
source), but the δ13C value for composition of the invention
generally, but not necessarily, ranges between -9.Salinity. to
-35.Salinity.. In some embodiments, the δ13C value for the
CO2 sequestering additive is between -1.Salinity. and -50.Salinity.,
between -5.Salinity. and -40.Salinity., between -5.Salinity. and
-35.Salinity., between -7.Salinity. and -40.Salinity., between
-7.Salinity. and -35.Salinity., between -9.Salinity. and -40.Salinity.,
or between -9.Salinity. and -35.Salinity.. In some embodiments, the
δ13C value for the CO2 sequestering additive is less than
(i.e., more negative than) -3.Salinity., -5.Salinity., -6.Salinity.,
-7.Salinity., -8.Salinity., -9.Salinity., -10.Salinity., -11.Salinity.,
-12.Salinity., -13.Salinity., -14.Salinity., -15.Salinity.,
-16.Salinity., -17.Salinity., -18.Salinity., -19.Salinity.,
-20.Salinity., -21.Salinity., -22.Salinity., -23.Salinity.,
-24.Salinity., -25.Salinity., -26.Salinity., -27.Salinity.,
-28.Salinity., -29.Salinity., -30.Salinity., -31.Salinity.,
-32.Salinity., -33.Salinity., -34.Salinity., -35.Salinity.,
-36.Salinity., -37.Salinity., -38.Salinity., -39.Salinity.,
-40.Salinity., -41.Salinity., -42.Salinity., -43.Salinity.,
-44.Salinity., or -45.Salinity., wherein the more negative the
δ13C value, the more rich the synthetic carbonate-containing
composition is in 12C. Any suitable method may be used for measuring
the δ13C value, methods including, but no limited to, mass
spectrometry or off-axis integrated-cavity output spectroscopy (off-axis
ICOS).

[0035] The compositions of the invention may vary greatly. By
non-cementitious is meant that the compositions are not settable
compositions, e.g., hydraulic cements. As such, the compositions are not
dried compositions that, when combined with a setting fluid, such as
water, set to produce a solid product. Illustrative compositions
according to certain embodiments of the invention are now reviewed
further in greater detail. However, the below review of compositions is
not limiting on the invention, and is provided solely to further describe
exemplary embodiments of the invention.

Paper Products

[0036] The present invention includes novel formulations which incorporate
the CO2 sequestering composition into paper products. The term
"paper products" is employed to refer to a thin material that is suitable
for use in one or more of writing upon, printing upon or packaging and
includes products commonly known as paper, card stock, and paperboard.
Card stock is a type of paper that is thicker and more durable than paper
but more flexible than paperboard (e.g., cardboard). Paper products of
the invention are produced by pressing together moist fibers (e.g.,
cellulose, polymeric) in the form of a pulp composition and then drying
the pressed fibers to form sheets of varying thickness. Paper products of
the invention may be produced in accordance with traditional
manufacturing protocols with the exception that an amount of the CO2
sequestering composition is employed. In producing paper products of the
invention, an amount of the CO2 sequestering composition may be
employed as a filler, absorbent or colorant to the pulp composition. By
"colorant" is meant a compound that is able to impart a color to a
product. Since the CO2 sequestering precipitate of the invention is
inherently white in color, it is able to improve the white color of
already white paper products, and lighten the color of paper products
that are not white.

[0037] The pulp composition may be derived from components which include,
but are not limited to eucalyptus pulp, banana tree bark, banana
stem-fibers, cotton fibers, vulcanized polymers, cellulose fibers, animal
skin (e.g., calfskin, sheepskin, goatskin), papyrus, high density
polyethylene fibers, hemp, bamboo, grass, rags or pulp derived from the
wood of any suitable tree. The moisture content of the pulp composition
may vary, ranging from 5% to 10%, such as 6% and including 7%. In some
instances, the CO2 sequestering composition may be added to the pulp
composition as an absorbent in order to decrease the moisture content in
the paper.

[0038] The density of paper products of the invention may vary greatly.
The density of "paper" ranges from 100 kg/m3 to 1500 kg/m3,
such as 250 kg/m3 to 1250 kg/m3, including 500 kg/m3 to
800 kg/m3. The density of "papercard" or "card stock" ranges from
1500 kg/m3 to 3000 kg/m3, such as 1700 kg/m3 to 2500
kg/m3, and including 2000 kg/m3 to 2250 kg/m3. The density
of "paperboard" can be 3000 kg/m3 and denser, such as 3500
kg/m3 and denser, including 5000 kg/m3 and denser. The
thickness of paper products the invention may also vary greatly. The
thickness of "paper" ranges between 0.05 mm to 0.18 mm, such as 0.07 mm
to 0.18 mm and including 0.1 mm to 0.15 mm. The thickness of "papercard"
ranges between 0.18 mm to 0.25 mm, such as 0.18 mm to 0.2 mm and
including 0.19 mm The thickness of "paperboard" may be 0.25 mm and
thicker, such as 0.3 mm and thicker, and including 1 mm and thicker. The
weight of paper products of the invention may vary. By "weight" is meant
the mass of paper product per unit area, usually measured in g/m2.
The weight of "paper" may range between 20 g/m2 to 160 g/m2,
such as 60 g/m2 to 150 g/m2 and including 80 g/m2 to 120
g/m2. The weight of "papercard" may range between 160 g/m2 to
500 g/m2, such as 175 g/m2 to 400 g/m2 and including 200
to g/m2 to 300 g/m2. The weight of "paperboard" may range from
500 g/m2 and heavier, such as 750 g/m2 and heavier and
including 2000 g/m2 and heavier.

[0039] In manufacturing paper products of the invention, the pulp
composition precursors of the paper products may include one or more
additional components, such as sizing agents, additional fillers (e.g.,
clay, china) and pigments. The amount of CO2 sequestering additive
in the finished paper product may vary, and may be 1% by weight or more,
such as 3% by weight or more, including 5% by weight or more. During
manufacture, following production of the pulp with the CO2
sequestering additive, the pulp may be pressed, dried and cut as desired
to produce a product of desired dimensions. The paper may also be
modified (e.g., bleached, treated with a sizing agent or surface coating)
after the finished paper product has been produced.

Polymeric Products

[0040] The present invention also includes novel formulations which
incorporate the CO2 sequestering composition into polymeric
products. The CO2 sequestering additive may be present in the
polymeric product in various amounts, as desired, and may be present as
fillers and/or other purposes. As such, the amount of CO2
sequestering additive in the polymeric composition may vary, and may be
1% by weight or more, such as 3% by weight or more, including 5% by
weight or more. In certain embodiments, the polymeric products are
plastics. The term "plastic" is used in its common sense to refer to a
wide range of synthetic or semisynthetic organic solid materials suitable
for the manufacture of industrial products (e.g., films, fibers, plates,
tubes, bottles, boxes). Plastics may be polymers of high molecular
weight, and may contain other substances to improve performance which may
include but are not limited to acid scavengers, antimicrobial agents,
antioxidants, antistatic agents, antifungal agents, clarifying agents,
flame retardants, amine light stabilizers, UV absorbers, optical
brighteners, photoselective additives, processing stabilizers, and the
like. Plastics of the invention may be acrylics, polyesters, silicones,
polyurethanes or halogenated plastics. Plastics of interest include, but
are not limited to: polypropylenes (e.g., as employed in food containers,
appliances, car bumpers), polystyrenes (e.g., as employed in packaging
foam, food containers, disposable cups, plates, cutlery, CD and cassette
boxes), high impact polystyrenes (e.g., as employed in fridge liners,
food packaging, vending cups), acrylonitrile butadiene styrene (e.g., as
employed in electronic equipment cases such as computer monitors,
printers, keyboards), polyethylene terephthalates (e.g., as employed in
carbonated drinks bottles, jars, plastic film, microwavable packaging),
polyesters (e.g., as employed in fibers, textiles), polyamides (e.g., as
employed in fibers, toothbrush bristles, fishing line, under-the-hood car
engine mouldings), poly(vinyl chloride) (e.g., as employed in plumbing
pipes and guttering, shower curtains, window frames,
flooring),polyurethanes (e.g., as employed in cushioning foams, thermal
insulation foams, surface coatings, printing rollers) polycarbonates
(e.g., as employed in compact discs, eyeglasses, riot shields, security
windows, traffic lights, lenses), polyvinylidene chloride (e.g., as
employed in food packaging, saran), polyethylene (e.g., as employed in
supermarket bags, plastic bottles) and polycarbonate/acrylonitrile
butadiene styrene (e.g., as employed in car interior and exterior parts).
Polymeric products, such as plastics, of the invention may be prepared in
accordance with traditional manufacturing protocols for such
compositions, with the exception that an amount of CO2 sequestering
additive of the invention is employed. As such, an amount of the CO2
sequestering additive may be combined with other additives of the plastic
precursor composition or feed, and then molded, cast, extruded into the
final desired plastic product.

Lubricants

[0041] The present invention also includes novel formulations which
incorporate the CO2 sequestering composition into lubricants. The
CO2 sequestering composition may be present in the lubricants in
various amounts, as desired, and may be present as fillers and/or other
purposes. The amount of CO2 sequestering additive in the lubricant
may vary, and may be 1% by weight or more, such as 3% by weight or more,
including 5% by weight or more. The lubricating oil composition may be
formulated for commercial purposes for use in internal combustion
engines, such as gasoline and diesel engines, crankcase lubrication and
the like. The oil (sometimes referred to as "base oil") is an oil of
lubricating viscosity and is the primary liquid constituent of a
lubricant, into which additives and possibly other oils are blended to
produce the final lubricant (herein "lubricating composition"). A base
oil may be selected from natural (vegetable, animal or mineral) and
synthetic lubricating oils and mixtures thereof. It may range in
viscosity from light distillate mineral oils to heavy lubricating oils
such as gas engine oil, mineral lubricating oil, motor vehicle oil, and
heavy duty diesel oil. In some instances, the viscosity of the oil ranges
from 2 to 30 mm2s-1, such as 5 to 20 mm2s-1 at
100° C.

[0042] Natural oils include animal oils and vegetable oils, liquid
petroleum oils and hydrorefined, solvent-treated or acid-treated mineral
lubricating oils of the paraffinic, naphthenic and mixed
paraffinic-naphthenic types. Oils of lubricating viscosity derived from
coal or shale are also useful base oils. Synthetic lubricating oils
include hydrocarbon oils and halo-substituted hydrocarbon oils such as
polymerized and interpolymerized olefins (e.g., polybutylenes,
polypropylenes, propylene-isobutylene copolymers, chlorinated
polybutylenes, poly(1-hexenes), poly(1-octenes), poly(1-decenes));
alkylbenzenes (e.g., dodecylbenzenes, tetradecylbenzenes,
dinonylbenzenes, di(2-ethylhexyl)benzenes); polyphenyls (e.g., biphenyls,
terphenyls, alkylated polyphenols); and alkylated diphenyl ethers and
alkylated diphenyl sulfides and the derivatives; analogs and homologs
thereof. Alkylene oxide polymers and interpolymers and derivatives
thereof where the terminal hydroxyl groups have been modified, for
example by esterification or etherification, constitute another class of
known synthetic lubricating oils. Another suitable class of synthetic
lubricating oils comprises the esters of dicarboxylic acids. Esters
useful as synthetic oils also include those made from C5 to C12
monocarboxylic acids and polyols, and polyol ethers such as neopentyl
glycol, trimethylolpropane, pentaerythritol, dipentaerythritol and
tripentaerythritol. Silicon-based oils such as the polyalkyl-, polyaryl-,
polyakoxy-, or polyaryloxysiloxane oils and silicate oils comprise
another useful class of synthetic lubricants.

[0043] Unrefined, refined and rerefined oils can be used in the lubricants
of the present invention. Unrefined oils are those obtained directly from
a natural or synthetic source without further purification treatment. For
example, a shale oil obtained directly from retorting operations, a
petroleum oil obtained directly from distillation or ester oil obtained
directly from an esterification process and used without further
treatment would be an unrefined oil. Refined oils are similar to the
unrefined oils except they have been further treated in one or more
purification steps to improve one or more properties. Many such
purification techniques, such as distillation, solvent extraction, acid
or base extraction, filtration and percolation are known to those skilled
in the art. Rerefined oils are obtained by processes similar to those
used to obtain refined oils applied to refined oils which have been
already used in service. Such rerefined oils are also known as reclaimed
or reprocessed oils and often are additionally processed by techniques
for removal of spent additives and oil breakdown products. Also present
may be one or more co-additives. Known additives may be incorporated into
the lubricant composition together with the additives of the invention.
They may, for example, include dispersants; other detergents, e.g. single
or mixed detergent systems; rust inhibitors; anti-wear agents;
anti-oxidants; corrosion inhibitors; friction modifiers or friction
reducing agents; pour point depressants; anti-foaming agents; viscosity
modifiers; and surfactants. They can be combined in proportions known in
the art. Some additives can provide a multiplicity of effects; thus, for
example, a single additive may act as a dispersant and as an oxidation
inhibitor.

[0044] In certain instances, the additive is a dispersant. A dispersant is
an additive for a lubricant whose primary function is to hold solid and
liquid contaminants in suspension, thereby passivating them and reducing
engine deposits at the same time as reducing sludge depositions. Thus,
for example, a dispersant maintains in suspension oil-insoluble
substances that result from oxidation during use of the lubricant, thus
preventing sludge flocculation and precipitation or deposition on metal
parts of the engine. Dispersants are usually "ashless", being
non-metallic organic materials that form substantially no ash on
combustion, in contrast to metal-containing, and hence ash-forming,
materials. They comprise a long chain hydrocarbon with a polar head, the
polarity being derived from inclusion of, e.g. an O, P or N atom. The
hydrocarbon is an oleophilic group that confers oil-solubility, having
for example 40 to 500 carbon atoms. Thus, ashless dispersants may
comprise an oil-soluble polymeric hydrocarbon backbone having functional
groups that are capable of associating with particles to be dispersed.
Typically, the dispersants comprise amine, alcohol, amide, or ester polar
moieties attached to the polymer backbone often via a bridging group. The
ashless dispersant may be, for example, selected from oil-soluble salts,
esters, amino-esters, amides, imides, and oxazolines of long chain
hydrocarbon-substituted mono- and dicarboxylic acids or their anhydrides;
thiocarboxylate derivatives of long chain hydrocarbons; long chain
aliphatic hydrocarbons having a polyamine attached directly thereto, and
Mannich condensation products formed by condensing a long chain
substituted phenol with formaldehyde and polyalkylene polyamine, such as
described in U.S. Pat. No. 3,442,808. Dispersants include, for example,
derivatives of long chain hydrocarbon-substituted carboxylic acids,
examples being derivatives of high molecular weight
hydrocarbyl-substituted succinic acid.

[0045] A noteworthy group of dispersants are hydrocarbon-substituted
succinimides, made, for example, by reacting the above acids (or
derivatives) with a nitrogen-containing compound, advantageously a
polyalkylene polyamine, such as a polyethylene polyamine. Particularly
preferred are the reaction products of polyalkylene polyamines with
alkenyl succinic anhydrides, such as described in U.S. Pat. Nos.
3,202,678; 3,154,560; 3,172,892; 3,024,195, 3,024,237; 3,219,666; and
3,216,936; and BE-A-66,875 that may be post-treated to improve their
properties, such as borated (as described in U.S. Pat. Nos. 3,087,936 and
3,254,025) fluorinated and oxylated. For example, boration may be
accomplished by treating an acyl nitrogen-containing dispersant with a
boron compound selected from boron oxide, boron halides, boron acids and
esters of boron acids. Also of interest are Anti-Wear and Anti-Oxidant
Agents. Dihydrocarbyl dithiophosphate metal salts are frequently used in
lubricants as anti-wear and antioxidant agents. The metal may be an
alkali or alkaline earth metal, or aluminum, lead, tin, zinc, molybdenum,
manganese, nickel or copper. The zinc salts are most commonly used in
lubricating oil in amounts of 0.1 to 10, preferably 0.2 to 2, mass %,
based upon the total weight of the lubricant. They may be prepared in
accordance with known techniques by first forming a dihydrocarbyl
dithiophosphoric acid (DDPA), usually by reaction of one or more alcohols
or a phenol with P2S5 and then neutralising the formed DDPA
with a zinc compound. The zinc dihydrocarbyl dithiophosphates can be made
from mixed DDPA which in turn may be made from mixed alcohols.
Alternatively, multiple zinc dihydrocarbyl dithiophosphates can be made
and subsequently mixed. Lubricants of the invention may be prepared in
accordance with traditional manufacturing protocols for such
compositions, with the exception that an amount of CO2 sequestering
additive of the invention is employed. As such, an amount of the CO2
sequestering additive may be combined with other components of the
lubricant and combined into the final desired lubricant product.

Adhesives

[0046] The present invention also includes novel formulations which
incorporate the CO2 sequestering composition into adhesives. By
"adhesives" is meant compounds that adhere to a substrate or bond two
substrates together. Adhesives of the invention may be produced in
accordance with traditional manufacturing protocols with the exception
that an amount of the CO2 sequestering composition is employed. In
producing adhesives of the invention, an amount of the CO2
sequestering composition may be employed as colorants, fillers, and to
improve rheology and increase tensile strength.

[0047] The physical properties of adhesives of the invention may vary
greatly depending upon the type of chemical system employed and the
amount of the CO2 sequestering composition added. The viscosity may
range from 1.0 cP to 750000 cP, such as 100 cP to 10000 cP, including 500
cP to 5000 cP, and including 1500 cP to 3000 cP. The effective
temperature of the adhesive may range between -75° C. to
500° C., such as 0° C. to 200° C. and including
50° C. to 150° C. By "effective temperature" is meant the
temperature range in which the adhesive shows no significant changes in
its physical properties or utility (i.e., insignificant change in
substrate bonding). The tensile strength of the adhesive may range from
0.1 MPa to 75 MPa, such as 10 MPa to 50 MPa and including 15 to 35 MPa.
The elongation capacity of the adhesives may range from 1.0% to 150%,
such as 40% to 100% and including 50% to 75%.

[0048] When added, the CO2 sequestering composition may increase the
viscosity, the storage and loss moduli of the adhesive, and in some
instances, impart pseudoplasticity and thixotropy. The amount of CO2
sequestering composition in adhesives of the invention may vary, ranging
from 5 to 40% by weight, such as 5 to 25% by weight and including 10 to
15% by weight.

[0050] In some embodiments, adhesives of the invention may be liquid
compositions which employ a solvent. Exemplary solvents may include, but
are not limited to xylene, methanol, toluene, mineral spirits, acetone,
butyl acetate, brominated solvents, mixtures thereof, among others. The
amount of solvent comprises about 10% to 90% of the liquid composition,
such as 50% to 75%, including 60% to 70%. The liquid composition may be
applied by brushing, spraying, rolling, immersing the substrate into the
composition, or any other convenient method for applying a coating to a
surface. In some instances, depending on the amount of solvent, the
liquid adhesive composition may be employed as a caulk or sealant. In
other instances, the liquid adhesive composition may be dispensed using
an aerosol sprayer by formulating the adhesive with a suitable
propellant. Exemplary propellants include, but are not limited to
fluorinated propellants such as HFCs, hydrocarbons such as propane,
butane, isobutane, pentane, nitrogen, carbon dioxide and any compatible
mixtures thereof. The amount of propellant may vary, ranging from 10% to
30%, such as 15% to 25%, including 15% to 20%. The composiion, including
the sprayable propellant may be packaged into an aerosol by any
convenient protocol.

[0051] In other embodiments, adhesives of the invention may be viscous
liquids, gels, soft solids or powders. In producing the viscous liquid,
soft solid, solid and gel adhesives, the components may be blended and
mixed using any convenient protocol. Exemplary methods for blending the
components include but are not limited to banbury mixers, sigman blade
mixers, double arm mixers, vortexing mixers, mixers that employ
sonication, mixers that employ heavy agitation, among others. Solid, soft
solid and gel adhesives of the invention may then be further shaped by
extruding, rotary pressing, stamping, cutting, laminating or molding to
produce the final adhesive product. In manufacturing adhesives of the
invention, the above mentioned constituents may also include one or more
additional components, such as anti-foaming agents, wetting agents,
thickeners, plasticizers, antioxidants and metal chelating agents.
Tackifiers which increase the adhesion of the compositions in general or
for specific surfaces may also be added. Exemplary tackifiers include
polyterpene resins, gum rosin, rosin esters and other rosin derivatives,
oil-soluble phenolic resins, coumaroneindene resins and petroleum
hydrocarbon resins.

[0053] Adhesives of the invention may be compatible with use on a number
of different types of substrates including but not limited to ceramic,
glass, concrete, masonry, composite materials, metal, paper or
paperboard, plastic, porous surfaces, rubber, elastomer, textiles,
fabrics or wood.

Rubber

[0054] The present invention also includes novel formulations which
incorporate the CO2 sequestering composition into rubber. The term
"rubber" is used in its conventional sense to mean an elastic material of
varying chemical composition which comprise long thread-like molecules
and possess a flexibility in its molecular chain to allow for overall
material flexing and coiling. Rubber of the invention may be produced in
accordance with traditional manufacturing protocols with the exception
that an amount of the CO2 sequestering composition is employed. In
producing rubber of the invention, an amount of the CO2 sequestering
composition may be employed as colorants, fillers and to improve
workability of the raw rubber product. Rubber of the invention may be
natural or synthetic. The term "natural" refers to rubber in the form of
a hydrocarbon polymer of isoprene units derived from the milky colloidal
suspension from the sap of a rubber tree or other such plants. Synthetic
rubber may be derived from a number of different synthetic polymers
including, but not limited to poly-styrene-butadiene, polyisobutylene,
ethylene-propylene copolymer, polyneoprene, butadiene-acrylonitrile
copolymer, fluoroelastomers, polyurethane, polysulfide, polyacrylate
among others. Rubber of the invention may also include one or more
additives, which include a vulcanizing agent, a vulcanization
accelerator, a process oil, an anti-aging agent, an antioxidant and an
anti-ozonant. In producing rubber of the invention, the components may be
blended or mixed with the CO2 sequestering composition using any
convenient protocol. Exemplary methods for blending the compositions
include banbury mixers, sigman blade mixers, double-arm mixers, vortexing
mixers, mixers that employ sonication, mixers that employ heavy
agitation, among others. The rubber may be further shaped by rotary
pressing, extruding, stamping, cutting, molding or any other convenient
protocol into the final rubber product.

Chalk

[0055] The present invention also includes novel formulations which
incorporate the CO2 sequestering composition into chalk. The term
"chalk" is used in its conventional sense to refer to a marking element
usually in the form of a stick or block used for writing or drawing on a
rough surface. Chalk in the present invention is a mixture of an amount
of the CO2 sequestering composition with one or more thermosetting
synthetic binders which is further processed into the form of sticks or
blocks. Binders used in the production of chalk may be any conventional
thermosetting synthetic binder. Exemplary binders include uncured epoxy,
polyester, polyurethane or acrylic resins, or compatible mixtures
thereof. Sticks or blocks of chalk are produced by forming a uniform
mixture of the CO2 sequestering composition with the synthetic
binder and pressing it under high pressure at room temperature. The
procedure is preferably such that the mixture of components are processed
in an extrusion press, cooled and crushed to a fine particle size, such
as 100 microns or smaller, including 75 microns or smaller and preferably
60 microns or smaller. The pulverulent mixture of components obtained is
then pressed at room temperature and under a pressure sufficient to
consolidate the powder (e.g., 10-35 MPa) into sticks or blocks of chalky
and friable consistency. Smaller sticks or blocks may also be cut from
larger pre-pressed blocks. Colored chalk may also be produced using the
above described method, with the exception that a colorant (i.e., dye)
may be added to the CO2 sequestering composition and binder mixture.

Asphalt Products

[0056] The present invention also includes novel formulations which
incorporate the CO2 sequestering composition into asphalt products.
The term "asphalt" (i.e., bitumen) is used in its conventional sense to
refer to the natural or manufactured black or dark-colored solid,
semisolid or viscous material composed mainly of high moleculer weight
hydrocarbons derived from a cut in petroleum distillation after naptha,
gasoline, kerosene and other fractions have been removed from crude oil.

[0057] The molecular composition of asphalt products may vary. Asphalt
products of the invention may be composed of saturated and unsaturated
aliphatic and aromatic compounds that possess functional groups that
include, but are not limited to alcohol, carboxyl, phenolic, amino, thiol
functional groups. In an exemplary embodiment, asphalt products may be
80% carbon by weight, 10% hydrogen by weight, 6% sulfur by weight, 3%
total weight of oxygen and nitrogen; and may also include trace amounts
of various metals such as iron, nickel and vanadium. The molecular weight
of asphalt products may range from 0.2 kDa to 50 kDa, such as 1 kDa to 25
kDa, including 2 kDa to 10 kDa. Components of asphalts may be asphaltenes
(i.e., high molecular weight compounds that are insoluble in hexane or
heptane) or maltenes (i.e., lower molecular weight compounds that are
soluble in hexane or heptane). The amount of asphaltenes in asphalt
products may vary, ranging from 5% to 25% by weight, such as 10% to 20%,
and including 12% to 15%. In some embodiments, asphalt products of the
invention may also contain a polymeric additive to enhance workability,
viscoelasticity, and strain recovery. Exemplary polymeric additives
include polybutadiene, polyisoprene, ethylene/vinyl acetate copolymer,
polyacrylate, polymethacrylate, polychloroprene, etc. Asphalt products of
interest also include an amount of aggregate. Aggregate of the invention
may be any convenient aggregate material. The aggregate material may be
CO2 sequestering aggregates, for example as described in U.S. patent
application Ser. No. 12/475,378, titled "ROCK AND AGGREGATE, AND METHODS
OF MAKING AND USING THE SAME"; the disclosure of which is herein
incorporated by reference.

[0058] Asphalt products of the invention may be prepared in accordance
with traditional manufacturing protocols, with the exception that an
amount of the CO2 sequestering composition of the invention is
employed. The amount of CO2 sequestering additive, e.g., present in
the asphalt product may vary, and may be 1% by weight or more, such as 3%
by weight or more, including 5% by weight or more, such as 25% by weight
or more, 50% by weight or more, 75% by weight or more. As such, an amount
of the CO2 sequestering additive may be combined with other
components of the asphalt product (e.g., asphalt, aggregate, cutback
solvents, polymeric additives), and then mixed to produce the final
asphalt product.

Paint

[0059] The present invention also includes novel formulations which
incorporate the CO2 sequestering composition into paint. By "paint"
is meant any liquid, liquefiable, or mastic composition which, after
application to a substrate in a thin layer, is converted to an opaque
solid film. Paints may include one or more of the following components:
pigments, binders, solvents and additives. Pigments are granular solids
incorporated into the paint, e.g., to contribute color, toughness or
simply to reduce the cost of the paint. Pigments of interest include
natural and synthetic types. Natural pigments include various clays,
calcium carbonate, mica, silicas, and talcs. Synthetic pigments include
engineered molecules, calcined clays, blanc fix, precipitated calcium
carbonate, and synthetic silicas. Hiding pigments, in making paint
opaque, also protect the substrate from the harmful effects of
ultraviolet light. Hiding pigments include titanium dioxide, phthalo
blue, red iron oxide, and many others. Fillers are a special type of
pigment that serve to thicken the film, support its structure and simply
increase the volume of the paint. Fillers of interest include inert
materials, such as talc, lime, baryte, clay, etc. Floor paints that will
be subjected to abrasion may even contain fine quartz sand as a filler.
Not all paints include fillers. On the other hand some paints contain
very large proportions of pigment/filler and binder. The CO2
sequestering additive of the invention may be employed in place of all or
some of the above pigment components in a given paint. The binder, or
resin, is the actual film forming component of paint. The binder imparts
adhesion, binds the pigments together, and strongly influences such
properties as gloss potential, exterior durability, flexibility, and
toughness. Binders of interest include synthetic or natural resins such
as acrylics, polyurethanes, polyesters, melamine resins, epoxy, or oils,
etc. Solvents of interest may be present, e.g., to adjust the viscosity
of the paint. They may be volatile so as not to become part of the paint
film. Solvents may be included to control flow and application
properties, and affect the stability of the paint while in liquid state.
Solvents of interest include water, e.g., water-based paints and organic
solvents, e.g., aliphatics, aromatics, alcohols, and ketones. Organic
solvents such as petroleum distillate, esters, glycol ethers, and the
like find use. Additives of interest include additives to modify surface
tension, improve flow properties, improve the finished appearance,
increase wet edge, improve pigment stability, impart antifreeze
properties, control foaming, control skinning, etc. Other types of
additives include catalysts, thickeners, stabilizers, emulsifiers,
texturizers, adhesion promoters, UV stabilizers, flatteners (de-glossing
agents), biocides to fight bacterial growth, and the like.

[0060] Paint products of the invention may be prepared in accordance with
traditional manufacturing protocols with the exception that an amount of
CO2 sequestering additive of the invention is employed. The amount
of CO2 sequestering additive in the paint may vary, and may be 1% by
weight or more, such as 3% by weight or more, including 5% by weight or
more, such as 25% by weight or more. As such, an amount of the CO2
sequestering additive may be combined with other components of the paint
such as pigment, binder, solvent, additive and then mixed to produce the
final paint product.

[0062] The CO2 sequestering composition of the invention may be
employed in non-ingestible products as an abrasive, absorbent, buffering
agent, filler, anti-caking agent, colorant, opacifying agent,
UV-scattering agent or oral care agent. Traditional abrasives,
absorbents, buffering agents, fillers, colorants, anti-caking agents,
opacifying agents, UV-scattering agents or oral care agents that are
conventionally found in non-ingestible products may be substituted
entirely or a certain amount removed and replaced using the CO2
sequestering composition of the present invention. The CO2
sequestering composition used to replace traditional additives may be
present in amounts such as 1% by weight or more, such as 3% by weight or
more, including 5% by weight or more, such as 25% by weight or more, 50%
by weight or more, 75% by weight or more.

[0063] In some embodiments, the CO2 sequestering composition of the
invention may be employed in non-ingestible products as an abrasive. By
"abrasive" is meant a compound that contains an amount of roughness which
when used on a surface is able to abrade, smooth, buff, polish, grind and
the like. The roughness of the abrasive may vary, depending on the
particle sizes of the CO2 sequestering composition. In some
instances, the particle sizes of the CO2 sequestering composition
are small (≦0.5 micron) and may be incorporated into
non-ingestible products where only a mild abrasive is desired (e.g.,
bathroom cleaners, baby wipes). In other instances, the particle sizes of
the CO2 sequestering precipitate are large (≧5 micron) and
may be incorporated into non-ingestible products where a strong abrasive
is desired (e.g., bath soap, toothpaste). Exemplary non-ingestible
products of the invention employing the CO2 sequestering composition
as an abrasive include toothpaste, shoe polish, mouthwash, facial
cleansing soaps, exfoliating products, acne prevention wipes, bath soap,
bath wash, makeup remover, baby wipes, diaper rash products, bathroom
cleaners, powdered bleach and all purpose cleaners. In some embodiments,
the CO2 sequestering composition is employed as an abrasive for
paint removal, such as in processes employing blasting techniques wherein
the abrasive is suspended in a liquid and applied to a painted or coated
surface. The CO2 sequestering composition may be used as an abrasive
for paint removal in cases where the surfaces are delicate, such as
lightweight metal and plastic surfaces, in some embodiments of the
invention.

[0064] In other embodiments, the CO2 sequestering composition of the
invention may be employed in non-ingestible products as an absorbent. By
"absorbent" is meant a compound that possesses the capacity to absorb or
soak up liquids (i.e., drying agent). Exemplary non-ingestible products
of the invention employing the CO2 sequestering composition as an
absorbent include eyeshadow, blush, concealer, foundation, face powder,
sunscreen, sun-tan lotion, self tanning compositions, bronzers, baby
powder, diaper rash products, deodorants and antiperspirants.

[0067] In other embodiments, the CO2 sequestering composition of the
invention may be employed in non-ingestible products as a filler. By
"filler" is meant a non-reactive, solid ingredient used to dilute other
solids, or to increase the volume of a product. In some instances, the
CO2 sequestering composition may be used to dilute a potent active
ingredient, which may be present in very small amounts, so that the
product can be handled more easily. In other instances, the CO2
sequestering composition may be used to increase the volume of an
expensive ingredient without disturbing the main function of the product.
Exemplary non-ingestible products of the invention employing the CO2
sequestering composition as a filler include baby powder, foundation,
face powder, blush, eyeshadow, diaper rash products, concealer, laundry
detergent, dishwashing powder, rinse agents, fast-dry agents, room
deodorizing powders, bathroom cleaners and powdered bleach.

[0068] In other embodiments, the CO2 sequestering composition of the
invention may be employed in non-ingestible products as a colorant. By
"colorant" is meant a compound that is able to impart a color to a
product. Since the CO2 sequestering precipitate of the invention is
inherently white in color, it is able to improve the white color of
already white products, and lighten the color of those products that are
not white. Exemplary non-ingestible products of the invention employing
the CO2 sequestering composition as a filler include eyeshadow,
blush, concealer, foundation, face powder, sunscreens, sun-tan lotion,
self tanning compositions, bronzers, baby powder, acne treatment cream,
facial cleansing soap, exfoliating soap, antiperspirants, deodorants,
bath soap, bath wash, shaving cream, moisturizers, anti-wrinkle cream,
teeth whitening agents, lotions, anti-inch cream, anti-fungal cream,
toothpaste, shampoo, conditioner, hair mousse, hair colorants, laundry
detergent, dishwashing powders and room deodorizing products.

[0069] In other embodiments, the CO2 sequestering composition of the
invention may be employed in non-ingestible products as an opacifying
agent. By "opacifying agent" is meant a substance that reduces the clear
or transparent appearance of a product. The opacity of the non-ingestible
product may vary depending on the particle sizes of the CO2
sequestering composition. For substantially opaque materials (e.g.,
anti-wrinkle cream), large particle sizes may be used (≧1 micron).
For compositions where a less substantial opacity is desired, small
particles may be used (≦0.5 micron). Exemplary non-ingestible
products of the invention employing the CO2 sequestering composition
as an opacifying agent include anti-wrinkle cream, bronzer, sun-tan
lotion and self-tanning compositions.

[0070] In other embodiments, the CO2 sequestering composition of the
invention may be employed in non-ingestible products as an oral-care
agent. By "oral-care agent" is meant a compound that may be used to
polish teeth, reduce oral odor or otherwise cleanse or deodorize the
teeth and mouth. In addition to being a mild abrasive for polishing
teeth, the CO2 sequestering composition, when incorporated in
products used for oral hygiene, can buffer acids that facilitate tooth
decay and provide a whitening component to oral-care products. Exemplary
non-ingestible products of the invention employing the CO2
sequestering composition as an oral-care agent include toothpaste, teeth
whitening agents and mouthwash.

[0071] In other embodiments, the CO2 sequestering composition of the
invention may be employed in non-ingestible products as a UV-scattering
agent. By "UV-scattering agent" is meant a compound that can sufficiently
scatter UV light. Depending on the particle sizes of the CO2
sequestering precipitate, the amount of UV light (i.e., light having
wavelengths≦380 nm) that is scattered and thus unavailable for
absorption may vary. In some instances, the amount of UV light scattered
may be 10% or more, including 25% or more, such as 50% or more. In some
embodiments of the invention, the CO2 sequestering composition may
be the only component used to protect against UV radiation. In other
embodiments, the CO2 sequestering composition may be used in
combination with conventional UV absorbing compositions to protect
against UV radiation. Exemplary non-ingestible products of the invention
employing the CO2 sequestering composition as a UV-scattering agent
include sunscreen, face powder, blush and foundation.

[0072] The present invention also includes novel formulations which
incorporate the CO2 sequestering composition into ingestible
products. By "ingestible" is meant compositions that are taken orally,
even though they may not be digested, where ingestibles are formulated
for human consumption. Ingestibles of the invention may include food
products, vitamins, nutritional supplements, pharmaceuticals and mineral
fortified products.

[0073] Of interest are novel ingestible formulations which incorporate the
CO2 sequestering composition of the invention into food products.
Food products of the invention are any ingestible solids or liquids,
usually composed of carbohydrates, fats, water and/or proteins that are
consumed for nutrition or pleasure. In certain embodiments, the CO2
sequestering composition of the invention may be employed in food
products as a buffering agent, filler, anti-caking agent, colorant,
emulsifier or stabilizer. Traditional buffering agents, fillers,
anti-caking agents, colorants, emulsifiers and stabilizers conventionally
found in food products may be substituted entirely or a certain amount
removed and replaced by the CO2 sequestering compositions of the
present invention.

[0074] In some embodiments, the CO2 sequestering composition of the
invention may be employed in food products as a buffering agent. As
described above, the CO2 sequestering composition may act to
minimize pH changes caused by any acidic or basic components
traditionally used in formulations for these products or may be used to
maintain a suitable pH for taste. Exemplary food products of the
invention employing the CO2 sequestering composition as a buffering
agent include condiments, fat emulsions (e.g., salad dressings)
water-based flavored drinks (e.g., energy drinks, sports drinks,
electrolyte drinks), soybean products (e.g., soy sauce), processed
fruits, canned fruits, processed vegetables, canned vegetables, processed
meats, canned meats, beer, wine, cider, malt beverages and canned soups.

[0075] In other embodiments, the CO2 sequestering composition of the
invention may be employed in food products as a filler. As described
above, a filler is a non-reactive, solid ingredient used to dilute other
solids, or to increase the volume of a product. Exemplary food products
of the invention employing the CO2 sequestering composition as a
filler include seasonings, dairy-based products, confectionary
substances, baby food, baby formula, sweeteners, milk powders, edible
casings and milk substitutes.

[0076] In other embodiments, the CO2 sequestering composition of the
invention may be employed in food products as an anti-caking agent. As
described above, an anti-caking agent is used to prevent solid
compositions from forming large aggregates (i.e., clumps) and facilitates
a consistent granular or powdered composition. Exemplary food products of
the invention employing the CO2 sequestering composition as an
anti-caking agent include milk powders, baby formula, confectionary
substances, sweeteners and seasonings.

[0077] In other embodiments, the CO2 sequestering composition of the
invention may be employed in food products as an emulsifier. By
"emulsifier" is meant a substance that forms or maintains a uniform
mixture of two or more immiscible phases. In some instances, the CO2
sequestering composition can be used to form a mixture of oil and water
in food products. Exemplary food products of the invention employing the
CO2 sequestering composition as an emulsifier include fat emulsions
(e.g., salad dressings), broths and condiments.

[0078] In other embodiments, the CO2 sequestering composition of the
invention may be employed in food products as a colorant. As described
above, a colorant is a compound that is able to impart a color to a
product. Since the CO2 sequestering precipitate of the invention is
inherently white in color, it is able to improve the white color of
already white products, and lighten the color of those products that are
not white. Exemplary food products of the invention employing the
CO2 sequestering composition as a colorant include dairy based
products, milk substitutes, milk powder, sweeteners, seasonings, baby
formula, dried egg products and confectionary substances.

[0079] In other embodiments, the CO2 sequestering composition of the
invention may be employed in food products as a stabilizer. By
"stabilizer" is meant a substance that facilitates a uniform dispersion
of two or more immiscible substances. Exemplary food products of the
invention employing the CO2 sequestering composition as a stabilizer
include dairy based products, canned soups, milk substitutes, liquid whey
and condiments.

[0080] Also of interest are novel ingestible formulations which
incorporate the CO2 sequestering composition of the invention into
vitamins, nutritional supplements and pharmaceuticals. Vitamins,
nutritional supplements and pharmaceuticals of the invention may include
any ingestible solids or liquids that are not food products (as described
above) consumed for nutritional or medicinal purposes. In certain
embodiments, the CO2 sequestering composition of the invention may
be employed in vitamins, nutritional supplements and pharmaceuticals as
buffering agents, fillers, anti-caking agents, colorants, and binders. By
"binder" is meant a substance that is used to hold together ingredients
of a compressed tablet or cake. Vitamins, nutritional supplements and
pharmaceuticals of the invention may be in the form or a powder, syrup,
liquid, tablet, capsule with powder filling, liquid-gel capsule and the
like. Vitamins, nutritional supplements and pharmaceuticals may include,
but are not limited to over-the-counter medications, behind-the-counter
medications, prescription medications, liquid nutritional drinks,
nutritional powders, weight-loss supplements, multivitamins,
nutraceuticals, laxatives, antacids and the like. Traditional buffering
agents, fillers, anti-caking agents, colorants and binders conventionally
found in vitamins, nutritional supplements and pharmaceuticals may be
substituted entirely or a certain amount removed and replaced by the
CO2 sequestering compositions of the present invention.

[0081] An exemplary embodiment, depending upon the components in the water
and the gaseous stream used to generate the carbonate precipitate of the
invention (as described in detail below) include preparing the CO2
sequestering carbonate precipitate in tablet form for use as a dietary
supplement or as an antacid (e.g., calcium supplement). Substantially
pure calcium and magnesium carbonate precipitate provided by methods of
the invention may be further processed into tablets by any convenient
protocol. The CO2 sequestering carbonate precipitate may also be
incorporated into tablets containing multiple dietary supplements (e.g.,
multivitamin).

[0083] The present invention also includes novel formulations which
incorporate the CO2 sequestering composition into animal ingestible
products. By "animal ingestible" is meant compositions that are taken
orally and are formulated for non-human (e.g., livestock, pets)
consumption. Animal Ingestible products of the invention may include but
are not limited to animal food products, vitamins, nutritional
supplements and pharmaceuticals for animal consumption. Of interest are
novel animal-ingestible product formulations which employ the CO2
sequestering composition of the invention as buffering agents, fillers,
anti-caking agents, colorants, emulsifiers, stabilizers and binders into
food products, vitamins, nutritional supplements and pharmaceuticals
formulated for animal consumption. Traditional buffering agents, fillers,
anti-caking agents, colorants, emulsifiers, stabilizers and binders
conventionally found in animal-ingestible products may be substituted
entirely or a certain amount removed and replaced by the CO2
sequestering compositions of the present invention.

Agricultural Products

[0084] The present invention also includes novel formulations which
incorporate the CO2 sequestering composition into agricultural
products. By "agricultural products" is meant any composition that is
employed in cultivating land, raising crops or vegetation, farming, and
feeding, breeding, and raising livestock or any other activity associated
therewith. Agricultural products of the invention may be soil amendment
compositions (e.g., fertilizer, remediation), pest control (fungicides,
insecticides) or nutritional and/or medicinal ingestible compositions for
livestock (as detailed above). The CO2 sequestering composition of
the invention may be added to traditional agricultural products as a
supplement or entirely replace conventionally used agricultural products.

[0085] In some embodiments, the CO2 sequestering composition of the
invention is a soil amendment. By "soil amendment" is meant a composition
that aims to improve or remediate the desired properties of soil for
agricultural usage. In some instances the soil amendment is a fertilizer
to supply nutrients (e.g., calcium, magnesium) to the soil. In other
instances, the soil amendment is a buffering agent to reduce changes to
the pH of the soil. The CO2 sequestering composition of the
invention may be contacted with the soil in the form of a slurry or a
powder. The CO2 sequestering precipitate is either mixed with water
prior to being dispensed onto the surface of the soil or is dispensed as
a dry powder. Contacting the composition with the soil may be achieved
using any convenient protocol. It may be gravity fed or pumped through
hoses, spray nozzles or fixed sprayers to uniformly apply the
composition. In other instances, the CO2 soil stabilization
compositions of the invention may be poured from a reservoir or applied
manually without the use of any industrial machinery. The composition may
also be applied by releasing the composition at a depth within the soil
by pumping the composition beneath the surface of the soil to be treated
or by digging to a depth in the soil using conventional digging machinery
and further applying the composition. The composition is then mixed into
the soil. In any of the various treatments within the scope of the
present invention, the soil may be mixed in situ or may be temporarily
removed from the ground for mixing and then replaced. Mixing the soil
with the CO2 sequestering composition may be accomplished using any
convenient mixing equipment (e.g., rotary mixers, cement mixers, etc.).
The prepared CO2-sequestering composition and soil mixture is then
rotated and the entire mixture is blended in a uniform manner.

[0086] In other embodiments, the CO2 sequestering composition of the
invention may be incorporated into pesticides. The term "pesticide" is
used in its conventional sense to mean any compound that is used to
eliminate, control or inhibit the proliferation of any organism which has
characteristics that are regarded as injurious or unwanted. Pesticides of
the invention may include those formulations used against insects, fungi,
bacteria, rodents and the like. The CO2 sequestering composition may
be employed in pesticides to improve the pesticide action or to aid in
the application of the pesticide. For example, the CO2 sequestering
composition may be employed as a water absorbent or as a granulating
agent. In other instances, the composition may be employed as a
crop-dusting filler to facilitate the uniform distribution of the
pesticide on vegetation or crops. Pesticides of the invention may be
prepared using any conventional protocol with the exception that an
amount of the CO2 sequestering composition is added. The amount of
CO2 sequestering additive in the pesticide may vary, and may be 1%
by weight or more, such as 3% by weight or more, including 5% by weight
or more, such as 25% by weight or more. The CO2 sequestrating
composition may be incorporated into the pesticides during the
formulation of the pesticide or may be subsequently added to the finished
pesticide product. Incorporation of the composition into the pesticide
may be accomplished by mixing the composition with the pesticide and
rotating the mixture under agitation, vortex or sonication and blending
into a uniform pesticide product.

Environmental Remediation

[0087] The CO2 sequestering composition of the invention may also be
employed in environmental remediation. By "environmental remediation" is
meant the removal of pollution or contaminants from environmental media
such as soil, groundwater, sediment or water for the general protection
of human health and the environment.

[0088] In some embodiments, environmental remediation employing the
CO2 sequestering composition of the invention is forest soil
restoration. The application of the CO2 sequestering composition may
be employed in forest soil restoration for neutralizing acidic soil,
improving the calcium and magnesium content in soil, increasing the
biological activity of organically influenced soil horizons, intensifying
the nitrification process in the soil or stabilizing metal organic
complexes in order to decrease or prevent heavy-metal pollution. The
CO2 sequestering composition of the invention may be contacted with
the forest soil using any convenient protocol (as discussed above). It
may be applied using devices that are gravity fed or it can be pumped
through hoses, spray nozzles or fixed sprayers. The composition may also
be poured from a reservoir or applied manually without the use of any
industrial machinery. In some instances, the CO2 sequestering
composition may be dispensed from a helicopter or crop-dusting airplane.

[0089] In other embodiments, environmental remediation employing the
CO2 sequestering composition of the invention is the neutralization
of over-acidified water. By "acidified water" is meant a large body of
water (e.g., pond, lake) that has a pH below 6.5 under ambient conditions
and is often lower, such as 6.0 and including 5.0. The CO2
sequestering composition can be applied by any convenient protocol. In
some instances, the composition is applied as a slurry or as a finely
ground powder. Slurries are typically sprayed onto the water surface from
boats or from stations located on the water, whereas powder is dispensed
by helicopter or fixed-wing planes. The application of the CO2
sequestering composition may cause increases in pH that vary ranging from
1 to 4, including 2 to 4, such as 2.5 to 3.5. The amount of the CO2
sequestering composition applied to the acidified water may vary
considerably (depending on the size and location of the body of water and
the pH of the water) ranging from 0.1 kg to 100 kg or more, such as 1000
kg or more, including 10,000 kg or more.

Preparation of CO2 Sequestering Compositions

[0090] Aspects of the invention also include methods of preparing CO2
sequestering compositions. CO2 sequestering compositions may be
prepared by producing a CO2 sequestering additive, e.g., as
described above, and then preparing the composition from the component.
Each of these aspects of the invention will now be described in greater
detail.

[0091] A variety of different methods may be employed to prepare the
CO2 sequestering additive of the compositions of the invention.
CO2 sequestration protocols of interest include, but are not limited
to, those disclosed in U.S. patent application Ser. Nos. 12/126,776,
titled, "Hydraulic cements comprising carbonate compound compositions,"
filed 23 May 2008; Ser. No. 12/163,205, titled "DESALINATION METHODS AND
SYSTEMS THAT INCLUDE CARBONATE COMPOUND PRECIPITATION," filed 27 Jun.
2008; and Ser. No. 12/486,692, titled "METHODS AND SYSTEMS FOR UTILIZING
WASTE SOURCES OF METAL OXIDES" filed 17 Jun. 2009; Ser. No. 12/501,217,
titled "PRODUCTION OF CARBONATE-CONTAINING COMPOSITIONS FROM MATERIAL
COMPRISING METAL SILICATE," filed 10 Jul. 2009; and Ser. No. 12/557,492,
titled "CO2 COMMODITY TRADING SYSTEM AND METHOD," filed 10 Sep. 2009; as
well as International Application No. PCT/US08/88318, titled, "METHODS OF
SEQUESTERING CO2," filed 24 Dec. 2008; and PCT/US09/45722, titled
"ROCK AND AGGREGATE, AND METHODS OF MAKING AND USING THE SAME," filed 29
May 2009; as well as pending U.S. Provisional Patent Application Ser.
Nos. 61/081,299; 61/082,766; 61/088,347; 61/088,340; and 61/101,631; the
disclosures of which are herein incorporated by reference.

[0092] CO2 sequestering additives of the invention include carbonate
compositions that may be produced by precipitating a calcium and/or
magnesium carbonate composition from a water. The carbonate compound
compositions that make up the CO2 sequestering additives of the
invention include may metastable carbonate compounds that may be
precipitated from a water, such as a salt-water, as described in greater
detail below. The carbonate compound compositions of the invention
include precipitated crystalline and/or amorphous carbonate compounds.

[0093] In certain embodiments, the water from which the carbonate
precipitates are produced is a saltwater. In such embodiments, the
carbonate compound composition may be viewed as a saltwater derived
carbonate compound composition. As used herein, "saltwater-derived
carbonate compound composition" means a composition derived from
saltwater and made up of one or more different carbonate crystalline
and/or amorphous compounds with or without one or more hydroxide
crystalline or amorphous compounds. The term "saltwater" is employed in
its conventional sense to refer to a number of different types of aqueous
liquids other than fresh water, where the term "saltwater" includes
brackish water, sea water and brine (including man-made brines, e.g.,
geothermal plant wastewaters, desalination waste waters, etc), as well as
other salines having a salinity that is greater than that of freshwater.
Brine is water saturated or nearly saturated with salt and has a salinity
that is 50 ppt (parts per thousand) or greater. Brackish water is water
that is saltier than fresh water, but not as salty as seawater, having a
salinity ranging from 0.5 to 35 ppt. Seawater is water from a sea or
ocean and has a salinity ranging from 35 to 50 ppt. The saltwater source
from which the mineral composition of the cements of the invention is
derived may be a naturally occurring source, such as a sea, ocean, lake,
swamp, estuary, lagoon, etc., or a man-made source. In certain
embodiments, the saltwater source of the mineral composition is seawater.

[0094] While the present invention is described primarily in terms of
saltwater sources, in certain embodiments, the water employed in the
invention may be a mineral rich, e.g., calcium and/or magnesium rich,
freshwater source. The water employed in the process is one that includes
one or more alkaline earth metals, e.g., magnesium, calcium, etc, and is
another type of alkaline-earth-metal-containing water that finds use in
embodiments of the invention. Waters of interest include those that
include calcium in amounts ranging from 50 to 20,000 ppm, such as 100 to
10,0000 ppm and including 200 to 5000 ppm. Waters of interest include
those that include magnesium in amounts ranging from 50 to 20,000 ppm,
such as 200 to 10000 ppm and including 500 to 5000 ppm.

[0095] The saltwater-derived carbonate compound compositions of
embodiments of the cements are ones that are derived from a saltwater. As
such, they are compositions that are obtained from a saltwater in some
manner, e.g., by treating a volume of a saltwater in a manner sufficient
to produce the desired carbonate compound composition from the initial
volume of saltwater. The carbonate compound compositions of certain
embodiments are produced by precipitation from a water, e.g., a
saltwater, a water that includes alkaline earth metals, such as calcium
and magnesium, etc., where such waters are collectively referred to as
alkaline-earth-metal-containing waters.

[0096] The saltwater employed in methods may vary. As reviewed above,
saltwaters of interest include brackish water, sea water and brine, as
well as other salines having a salinity that is greater than that of
freshwater (which has a salinity of less than 5 ppt dissolved salts. In
some embodiments, calcium rich waters may be combined with magnesium
silicate minerals, such as olivine or serpentine, in solution that has
become acidic due to the addition on carbon dioxide to form carbonic
acid, which dissolves the magnesium silicate, leading to the formation of
calcium magnesium silicate carbonate compounds as mentioned above.

[0097] In methods of producing the carbonate compound compositions of the
aggregates of the invention, a volume of water is subjected to carbonate
compound precipitation conditions sufficient to produce a precipitated
carbonate compound composition and a mother liquor (i.e., the part of the
water that is left over after precipitation of the carbonate compound(s)
from the saltwater). The resultant precipitates and mother liquor
collectively make up the carbonate compound compositions of the
invention. Any convenient precipitation conditions may be employed, which
conditions result in the production of a carbonate compound composition
sequestration product.

[0098] Precipitation conditions of interest may vary. For example, the
temperature of the water may be within a suitable range for the
precipitation of the desired mineral to occur. In some embodiments, the
temperature of the water may be in a range from 5 to 70° C., such
as from 20 to 50° C. and including from 25 to 45° C. As
such, while a given set of precipitation conditions may have a
temperature ranging from 0 to 100° C., the temperature of the
water may have to be adjusted in certain embodiments to produce the
desired precipitate.

[0099] In normal sea water, 93% of the dissolved CO2 is in the form
of bicarbonate ions (HCO3.sup.-) and 6% is in the form of carbonate
ions (CO3-2). When calcium carbonate precipitates from normal
sea water, CO2 is released. In fresh water, above pH 10.33, greater
than 90% of the carbonate is in the form of carbonate ion, and no
CO2 is released during the precipitation of calcium carbonate. In
sea water this transition occurs at a slightly lower pH, closer to a pH
of 9.7. While the pH of the water employed in methods may range from 5 to
14 during a given precipitation process, in certain embodiments the pH is
raised to alkaline levels in order to drive the precipitation of
carbonate compounds, as well as other compounds, e.g., hydroxide
compounds, as desired. In certain of these embodiments, the pH is raised
to a level which minimizes if not eliminates CO2 production during
precipitation, causing dissolved CO2, e.g., in the form of carbonate
and bicarbonate, to be trapped in the carbonate compound precipitate. In
these embodiments, the pH may be raised to 10 or higher, such as 11 or
higher.

[0100] The pH of the water may be raised using any convenient approach. In
certain embodiments, a pH raising agent may be employed, where examples
of such agents include oxides, hydroxides (e.g., calcium oxide in fly
ash, potassium hydroxide, sodium hydroxide, brucite (Mg(OH2), etc.),
carbonates (e.g., sodium carbonate) and the like. One such approach is to
use the coal ash from a coal-fired power plant, which contains many
oxides, to elevate the pH of the water. Other coal processes, like the
gasification of coal, to produce syngas, also produce hydrogen gas and
carbon monoxide, and may serve as a source of hydroxide as well. Some
naturally occurring minerals, such as serpentine, contain hydroxide, and
can be dissolved, yielding a hydroxide source. The addition of
serpentine, also releases silica and magnesium into the solution, leading
to the formation of silica containing carbonate compounds. The amount of
pH elevating agent that is added to the water will depend on the
particular nature of the agent and the volume of water being modified,
and will be sufficient to raise the pH of the water to the desired value.
Alternatively, the pH of the water source can be raised to the desired
level by electrolysis of water. Where electrolysis is employed, a variety
of different protocols may be taken, such as use of the Mercury cell
process (also called the Castner-Kellner process); the Diaphragm cell
process and the membrane cell process. Where desired, byproducts of the
hydrolysis product, e.g., H2, sodium metal, etc. may be harvested
and employed for other purposes, as desired. In some embodiments,
described further below, HCl is a byproduct of the process and may be
used, e.g. in the manufacture of poly (vinyl chloride) (PVC).

[0101] Methods of the invention include contacting a volume of an aqueous
solution of divalent cations with a source of CO2 (to dissolve
CO2) and subjecting the resultant solution to precipitation
conditions. In some embodiments, a volume of an aqueous solution of
divalent cations is contacted with a source of CO2 (to dissolve
CO2) while subjecting the aqueous solution to precipitation
conditions. The dissolution of CO2 into the aqueous solution of
divalent cations produces carbonic acid, a species in equilibrium with
both bicarbonate and carbonate. In order to produce carbonate-containing
precipitation material, protons are removed from various species (e.g.
carbonic acid, bicarbonate, hydronium, etc.) in the divalent
cation-containing solution to shift the equilibrium toward carbonate. As
protons are removed, more CO2 goes into solution. In some
embodiments, proton-removing agents and/or methods are used while
contacting a divalent cation-containing aqueous solution with CO2 to
increase CO2 absorption in one phase of the precipitation reaction,
wherein the pH may remain constant, increase, or even decrease, followed
by a rapid removal of protons (e.g., by addition of a base) to cause
rapid precipitation of carbonate-containing precipitation material.
Protons may be removed from the various species (e.g. carbonic acid,
bicarbonate, hydronium, etc.) by any convenient approach, including, but
not limited to use of naturally occurring proton-removing agents, use of
microorganisms and fungi, use of synthetic chemical proton-removing
agents, recovery of man-made waste streams, and using electrochemical
means.

[0102] Naturally occurring proton-removing agents encompass any
proton-removing agents that can be found in the wider environment that
may create or have a basic local environment. Some embodiments provide
for naturally occurring proton-removing agents including minerals that
create basic environments upon addition to solution. Such minerals
include, but are not limited to, lime (CaO); periclase (MgO); iron
hydroxide minerals (e.g., goethite and limonite); and volcanic ash.
Methods for digestion of such minerals and rocks comprising such minerals
are provided herein. Some embodiments provide for using naturally
alkaline bodies of water as naturally occurring proton-removing agents.
Examples of naturally alkaline bodies of water include, but are not
limited to surface water sources (e.g. alkaline lakes such as Mono Lake
in California) and ground water sources (e.g. basic aquifers such as the
deep geologic alkaline aquifers located at Searles Lake in California).
Other embodiments provide for use of deposits from dried alkaline bodies
of water such as the crust along Lake Natron in Africa's Great Rift
Valley. In some embodiments, organisms that excrete basic molecules or
solutions in their normal metabolism are used as proton-removing agents.
Examples of such organisms are fungi that produce alkaline protease
(e.g., the deep-sea fungus Aspergillus ustus with an optimal pH of 9) and
bacteria that create alkaline molecules (e.g., cyanobacteria such as
Lyngbya sp. from the Atlin wetland in British Columbia, which increases
pH from a byproduct of photosynthesis). In some embodiments, organisms
are used to produce proton-removing agents, wherein the organisms (e.g.,
Bacillus pasteurii, which hydrolyzes urea to ammonia) metabolize a
contaminant (e.g. urea) to produce proton-removing agents or solutions
comprising proton-removing agents (e.g., ammonia, ammonium hydroxide). In
some embodiments, organisms are cultured separately from the
precipitation reaction mixture, wherein proton-removing agents or
solution comprising proton-removing agents are used for addition to the
precipitation reaction mixture. In some embodiments, naturally occurring
or manufactured enzymes are used in combination with proton-removing
agents to invoke precipitation of precipitation material. Carbonic
anhydrase, which is an enzyme produced by plants and animals, accelerates
transformation of carbonic acid to bicarbonate in aqueous solution.

[0103] Chemical agents for effecting proton removal generally refer to
synthetic chemical agents that are produced in large quantities and are
commercially available. For example, chemical agents for removing protons
include, but are not limited to, hydroxides, organic bases, super bases,
oxides, ammonia, and carbonates. Hydroxides include chemical species that
provide hydroxide anions in solution, including, for example, sodium
hydroxide (NaOH), potassium hydroxide (KOH), calcium hydroxide
(Ca(OH)2), or magnesium hydroxide (Mg(OH)2). Organic bases are
carbon-containing molecules that are generally nitrogenous bases
including primary amines such as methyl amine, secondary amines such as
diisopropylamine, tertiary such as diisopropylethylamine, aromatic amines
such as aniline, heteroaromatics such as pyridine, imidazole, and
benzimidazole, and various forms thereof. In some embodiments, an organic
base selected from pyridine, methylamine, imidazole, benzimidazole,
histidine, and a phophazene is used to remove protons from various
species (e.g., carbonic acid, bicarbonate, hydronium, etc.) for
precipitation of precipitation material. In some embodiments, ammonia is
used to raise pH to a level sufficient to precipitate precipitation
material from a solution of divalent cations and an industrial waste
stream. Super bases suitable for use as proton-removing agents include
sodium ethoxide, sodium amide (NaNH2), sodium hydride (NaH), butyl
lithium, lithium diisopropylamide, lithium diethylamide, and lithium
bis(trimethylsilyl)amide. Oxides including, for example, calcium oxide
(CaO), magnesium oxide (MgO), strontium oxide (SrO), beryllium oxide
(BeO), and barium oxide (BaO) are also suitable proton-removing agents
that may be used. Carbonates for use in the invention include, but are
not limited to, sodium carbonate.

[0104] In addition to comprising cations of interest and other suitable
metal forms, waste streams from various industrial processes may provide
proton-removing agents. Such waste streams include, but are not limited
to, mining wastes; fossil fuel burning ash (e.g., combustion ash such as
fly ash, bottom ash, boiler slag); slag (e.g. iron slag, phosphorous
slag); cement kiln waste; oil refinery/petrochemical refinery waste (e.g.
oil field and methane seam brines); coal seam wastes (e.g. gas production
brines and coal seam brine); paper processing waste; water softening
waste brine (e.g., ion exchange effluent); silicon processing wastes;
agricultural waste; metal finishing waste; high pH textile waste; and
caustic sludge. Mining wastes include any wastes from the extraction of
metal or another precious or useful mineral from the earth. In some
embodiments, wastes from mining are used to modify pH, wherein the waste
is selected from red mud from the Bayer aluminum extraction process;
waste from magnesium extraction from sea water (e.g., Mg(OH)2 such
as that found in Moss Landing, Calif.); and wastes from mining processes
involving leaching. For example, red mud may be used to modify pH as
described in U.S. Provisional Patent Application No. 61/161,369, titled,
"NEUTRALIZING INDUSTRIAL WASTES UTILIZING CO2 AND A DIVALENT CATION
SOLUTION", filed 18 Mar. 2009, which is hereby incorporated by reference
in its entirety. Fossil fuel burning ash, cement kiln dust, and slag,
collectively waste sources of metal oxides, further described in U.S.
patent application Ser. No. 12/486,692, titled, "METHODS AND SYSTEMS FOR
UTILIZING WASTE SOURCES OF METAL OXIDES," filed 17 Jun. 2009, the
disclosure of which is incorporated herein in its entirety, may be used
in alone or in combination with other proton-removing agents to provide
proton-removing agents for the invention. Agricultural waste, either
through animal waste or excessive fertilizer use, may contain potassium
hydroxide (KOH) or ammonia (NH3) or both. As such, agricultural
waste may be used in some embodiments of the invention as a
proton-removing agent. This agricultural waste is often collected in
ponds, but it may also percolate down into aquifers, where it can be
accessed and used.

[0105] Electrochemical methods are another means to remove protons from
various species in a solution, either by removing protons from solute
(e.g., deprotonation of carbonic acid or bicarbonate) or from solvent
(e.g., deprotonation of hydronium or water). Deprotonation of solvent may
result, for example, if proton production from CO2 dissolution
matches or exceeds electrochemical proton removal from solute molecules.
In some embodiments, low-voltage electrochemical methods are used to
remove protons, for example, as CO2 is dissolved in the
precipitation reaction mixture or a precursor solution to the
precipitation reaction mixture (i.e., a solution that may or may not
contain divalent cations). In some embodiments, CO2 dissolved in an
aqueous solution that does not contain divalent cations is treated by a
low-voltage electrochemical method to remove protons from carbonic acid,
bicarbonate, hydronium, or any species or combination thereof resulting
from the dissolution of CO2. A low-voltage electrochemical method
operates at an average voltage of 2, 1.9, 1.8, 1.7, or 1.6 V or less,
such as 1.5, 1.4, 1.3, 1.2, 1.1 V or less, such as 1 V or less, such as
0.9 V or less, 0.8 V or less, 0.7 V or less, 0.6 V or less, 0.5 V or
less, 0.4 V or less, 0.3 V or less, 0.2 V or less, or 0.1 V or less.
Low-voltage electrochemical methods that do not generate chlorine gas are
convenient for use in systems and methods of the invention. Low-voltage
electrochemical methods to remove protons that do not generate oxygen gas
are also convenient for use in systems and methods of the invention. In
some embodiments, low-voltage electrochemical methods generate hydrogen
gas at the cathode and transport it to the anode where the hydrogen gas
is converted to protons. Electrochemical methods that do not generate
hydrogen gas may also be convenient. In some embodiments, electrochemical
processes to remove protons do not generate a gas at the anode. In some
instances, electrochemical methods to remove protons do not generate any
gaseous by-byproduct. Electrochemical methods for effecting proton
removal are further described in U.S. patent application Ser. No.
12/344,019, titled, "METHODS OF SEQUESTERING CO2," filed 24 Dec.
2008; U.S. patent application Ser. No. 12/375,632, titled, "LOW ENERGY
ELECTROCHEMICAL HYDROXIDE SYSTEM AND METHOD," filed 23 Dec. 2008;
International Patent Application No. PCT/US08/088242, titled, "LOW ENERGY
ELECTROMECHANICAL HYDROXIDE SYSTEM AND METHOD," filed 23 Dec. 2008;
International Patent Application No. PCT/US09/32301, titled, "LOW-ENERGY
ELECTROCHEMICAL BICARBONATE ION SOLUTION," filed 28 Jan. 2009; and
International Patent Application No. PCT/US09/48511, titled, "LOW-ENERGY
4-CELL ELECTROCHEMICAL SYSTEM WITH CARBON DIOXIDE GAS," filed 24 Jun.
2009, each of which are incorporated herein by reference in their
entirety.

[0106] Low voltage electrochemical processes may produce hydroxide at the
cathode and protons at the anode; where such processes utilize a salt
containing chloride, e.g. NaCl, a product of the process will be HCl. In
some embodiments of the invention, the HCL from a low-voltage
electrochemical process as described herein may be used to make
poly(vinyl chloride) (PVC). HCl from a low-voltage electrochemical
process, e.g. a process that operates at a voltage of less than 2.0V, or
less than 1.5V, or less than 1.0V, may be used in reactions well-known in
the art to produce a vinyl chloride monomer. The vinyl chloride monomer
may be used to produce poly(vinyl chloride) in some embodiments. In
further embodiments, the PVC can be mixed with a carbonate precipitate
formed by the methods described herein, e.g. a slightly wet carbonate
precipitate, to form a building material. In some embodiments, the
PVC/carbonate mixture may be extruded to form a slightly foamed profile,
such as, e.g. a 2×4 or other lumber material. Carbonate/PVC lumber
formed by such methods are thus encompassed by the invention. Such 1
umber may be CO2-sequestering because the carbonate in the lumber is
a CO2-sequestering additive. In some embodiments, the amount of
CO2 sequestering additive in the formed element comprising PVC is 5
wt % or more. In some embodiments, the amount of CO2 sequestering
additive in the formed element comprising PVC is 10 wt % or more, 15 wt %
or more, 20 wt % or more, 25 wt % or more, 30 wt % or more, 35 wt % or
more, such as 40 wt % or more, 45 wt % or more, 50 wt %, 55 wt % or more,
60 wt % or more, such as up to 65 wt % or more. In some embodiments, the
amount of CO2 sequestering additive in the formed element comprising
PVC is 60 wt % or more. In some embodiments, the PVC and CO2
sequestering additive are mixed and formed in a screw extruder. In some
embodiments, the formed element is injection molded. In some embodiments,
the PVC is foamed to create a cellular structure that will hold anchoring
devices such as nails and screws. In some embodiments, the formed element
comprising PVC and CO2 sequestering additive is used to fabricate
building elements that are flame resistant. In some embodiments, the
formed element comprising PVC and CO2 sequestering additive is such
that the amount of CO2 sequestering additive increases the
finishability, i.e. ease of cutting and sanding, of the formed element.
In some embodiments, the formed element comprising PVC and CO2
sequestering additive is such that the amount of CO2 sequestering
additive enhances the coloring or appearance of the formed element. In
some embodiments, the formed element comprising PVC and CO2
sequestering additive is such that the amount of CO2 sequestering
additive gives stiffness to the formed element. In some embodiments, the
CO2 sequestering additive is added to the PVC during the production
of the PVC. In some such embodiments, the PVC can be derived from the
CO2 sequestering methods of the invention.

[0107] Alternatively, electrochemical methods may be used to produce
caustic molecules (e.g., hydroxide) through, for example, the
chlor-alkali process, or modification thereof. Electrodes (i.e., cathodes
and anodes) may be present in the apparatus containing the divalent
cation-containing aqueous solution or gaseous waste stream-charged (e.g.,
CO2-charged) solution, and a selective barrier, such as a membrane,
may separate the electrodes. Electrochemical systems and methods for
removing protons may produce by-products (e.g., hydrogen) that may be
harvested and used for other purposes. Additional electrochemical
approaches that may be used in systems and methods of the invention
include, but are not limited to, those described in U.S. patent
application Ser. No. 12/503,557, titled, "CO2 UTILIZATION IN
ELECTROCHEMICAL SYSTEMS," filed 15 Jul. 2009 and U.S. Provisional
Application No. 61/091,729, titled, "LOW ENERGY ABSORPTION OF HYDROGEN
ION FROM AN ELECTROLYTE SOLUTION INTO A SOLID MATERIAL," filed 11 Sep.
2008, the disclosures of which are herein incorporated by reference.

[0108] Combinations of the above mentioned sources of proton removal may
be employed. One such combination is the use of a microorganisms and
electrochemical systems. Combinations of microorganisms and
electrochemical systems include microbial electrolysis cells, including
microbial fuel cells, and bio-electrochemically assisted microbial
reactors. In such microbial electrochemical systems, microorganisms (e.g.
bacteria) are grown on or very near an electrode and in the course of the
metabolism of material (e.g. organic material) electrons are generated
that are taken up by the electrode.

[0109] Additives other than pH elevating agents may also be introduced
into the water in order to influence the nature of the precipitate that
is produced. As such, certain embodiments of the methods include
providing an additive in water before or during the time when the water
is subjected to the precipitation conditions. Certain calcium carbonate
polymorphs can be favored by trace amounts of certain additives. For
example, vaterite, a highly unstable polymorph of CaCO3 which
precipitates in a variety of different morphologies and converts rapidly
to calcite, can be obtained at very high yields by including trace
amounts of lanthanum as lanthanum chloride in a supersaturated solution
of calcium carbonate. Other additives beside lanthanum that are of
interest include, but are not limited to transition metals and the like.
For instance, the addition of ferrous or ferric iron is known to favor
the formation of disordered dolomite (protodolomite) where it would not
form otherwise.

[0110] The nature of the precipitate can also be influenced by selection
of appropriate major ion ratios. Major ion ratios also have considerable
influence of polymorph formation. For example, as the magnesium:calcium
ratio in the water increases, aragonite becomes the favored polymorph of
calcium carbonate over low-magnesium calcite. At low magnesium:calcium
ratios, low-magnesium calcite is the preferred polymorph. As such, a wide
range of magnesium:calcium ratios can be employed, including, e.g.,
100/1, 50/1, 20/1, 10/1, 5/1, 2/1, 1/1, 1/2, 1/5, 1/10, 1/20, 1/50,
1/100. In certain embodiments, the magnesium:calcium ratio is determined
by the source of water employed in the precipitation process (e.g.,
seawater, brine, brackish water, fresh water), whereas in other
embodiments, the magnesium:calcium ratio is adjusted to fall within a
certain range.

[0111] Rate of precipitation also has a large effect on compound phase
formation. The most rapid precipitation can be achieved by seeding the
solution with a desired phase. Without seeding, rapid precipitation can
be achieved by rapidly increasing the pH of the sea water, which results
in more amorphous constituents. When silica is present, the more rapid
the reaction rate, the more silica is incorporated with the carbonate
precipitate. The higher the pH is, the more rapid the precipitation is
and the more amorphous the precipitate is.

[0112] Accordingly, a set of precipitation conditions to produce a desired
precipitate from a water include, in certain embodiments, the water's
temperature and pH, and in some instances the concentrations of additives
and ionic species in the water. Precipitation conditions may also include
factors such as mixing rate, forms of agitation such as ultrasonics, and
the presence of seed crystals, catalysts, membranes, or substrates. In
some embodiments, precipitation conditions include supersaturated
conditions, temperature, pH, and/or concentration gradients, or cycling
or changing any of these parameters. The protocols employed to prepare
carbonate compound precipitates according to the invention may be batch
or continuous protocols. It will be appreciated that precipitation
conditions may be different to produce a given precipitate in a
continuous flow system compared to a batch system.

[0113] In certain embodiments, the methods further include contacting the
volume of water that is subjected to the mineral precipitation conditions
with a source of CO2. Contact of the water with the source CO2
may occur before and/or during the time when the water is subjected to
CO2 precipitation conditions. Accordingly, embodiments of the
invention include methods in which the volume of water is contacted with
a source of CO2 prior to subjecting the volume of saltwater to
mineral precipitation conditions. Embodiments of the invention include
methods in which the volume of salt water is contacted with a source of
CO2 while the volume of saltwater is being subjected to carbonate
compound precipitation conditions. Embodiments of the invention include
methods in which the volume of water is contacted with a source of a
CO2 both prior to subjecting the volume of saltwater to carbonate
compound precipitation conditions and while the volume of saltwater is
being subjected to carbonate compound precipitation conditions. In some
embodiments, the same water may be cycled more than once, wherein a first
cycle of precipitation removes primarily calcium carbonate and magnesium
carbonate minerals, and leaves remaining alkaline water to which other
alkaline earth ion sources may be added, that can have more carbon
dioxide cycled through it, precipitating more carbonate compounds.

[0114] The source of CO2 that is contacted with the volume of
saltwater in these embodiments may be any convenient CO2 source. The
CO2 source may be a liquid, solid (e.g., dry ice) or gaseous
CO2 source. In certain embodiments, the CO2 source is a gaseous
CO2 source. This gaseous CO2 is, in certain instances, a waste
feed from an industrial plant. The nature of the industrial plant may
vary in these embodiments, where industrial plants of interest include
power plants (e.g., as described in further detail in International
Application No. PCT/US08/88318, titled, "METHODS OF SEQUESTERING
CO2," filed 24 Dec. 2008, the disclosure of which is herein
incorporated by reference), chemical processing plants, steel mills,
paper mills, cement plants (e.g., as described in further detail in U.S.
Provisional Application Ser. No. 61/088,340, the disclosure of which is
herein incorporated by reference), and other industrial plants that
produce CO2 as a byproduct. By waste feed is meant a stream of gas
(or analogous stream) that is produced as a byproduct of an active
process of the industrial plant. The gaseous stream may be substantially
pure CO2 or a multi-component gaseous stream that includes CO2
and one or more additional gases. Multi-component gaseous streams
(containing CO2) that may be employed as a CO2 source in
embodiments of the subject methods include both reducing, e.g., syngas,
shifted syngas, natural gas, and hydrogen and the like, and oxidizing
condition streams, e.g., flue gases from combustion. Exhaust gases
containing NOx, SOx, VOCs, particulates and Hg would commonly incorporate
these compounds along with the carbonate in the precipitated product.
Particular multi-component gaseous streams of interest that may be
treated according to the subject invention include: oxygen containing
combustion power plant flue gas, turbo charged boiler product gas, coal
gasification product gas, shifted coal gasification product gas,
anaerobic digester product gas, wellhead natural gas stream, reformed
natural gas or methane hydrates, and the like.

[0115] The volume of saltwater may be contacted with the CO2 source
using any convenient protocol. Where the CO2 is a gas, contact
protocols of interest include, but are not limited to: direct contacting
protocols, e.g., bubbling the gas through the volume of saltwater,
concurrent contacting means, i.e., contact between unidirectionally
flowing gaseous and liquid phase streams, countercurrent means, i.e.,
contact between oppositely flowing gaseous and liquid phase streams, and
the like. Thus, contact may be accomplished through use of infusers,
bubblers, fluidic Venturi reactor, sparger, gas filter, spray, tray, or
packed column reactors, and the like, as may be convenient.

[0116] The above protocol results in the production of a slurry of a
CO2 sequestering precipitate and a mother liquor. Where desired, the
compositions made up of the precipitate and the mother liquor may be
stored for a period of time following precipitation and prior to further
processing. For example, the composition may be stored for a period of
time ranging from 1 to 1000 days or longer, such as 1 to 10 days or
longer, at a temperature ranging from 1 to 40° C., such as 20 to
25° C.

[0117] The slurry components are then separated. Embodiments may include
treatment of the mother liquor, where the mother liquor may or may not be
present in the same composition as the product. For example, where the
mother liquor is to be returned to the ocean, the mother liquor may be
contacted with a gaseous source of CO2 in a manner sufficient to
increase the concentration of carbonate ion present in the mother liquor.
Contact may be conducted using any convenient protocol, such as those
described above. In certain embodiments, the mother liquor has an
alkaline pH, and contact with the CO2 source is carried out in a
manner sufficient to reduce the pH to a range between 5 and 9, e.g., 6
and 8.5, including 7.5 to 8.2. In certain embodiments, the treated brine
may be contacted with a source of CO2, e.g., as described above, to
sequester further CO2. For example, where the mother liquor is to be
returned to the ocean, the mother liquor may be contacted with a gaseous
source of CO2 in a manner sufficient to increase the concentration
of carbonate ion present in the mother liquor. Contact may be conducted
using any convenient protocol, such as those described above. In certain
embodiments, the mother liquor has an alkaline pH, and contact with the
CO2 source is carried out in a manner sufficient to reduce the pH to
a range between 5 and 9, e.g., 6 and 8.5, including 7.5 to 8.2.

[0118] The resultant mother liquor of the reaction may be disposed of
using any convenient protocol. In certain embodiments, it may be sent to
a tailings pond for disposal. In certain embodiments, it may be disposed
of in a naturally occurring body of water, e.g., ocean, sea, lake or
river. In certain embodiments, the mother liquor is returned to the
source of feedwater for the methods of invention, e.g., an ocean or sea.
Alternatively, the mother liquor may be further processed, e.g.,
subjected to desalination protocols, as described further in U.S.
application Ser. No. 12/163,205; the disclosure of which is herein
incorporated by reference.

[0119] In certain embodiments, following production of the CO2
sequestering product, the resultant product is separated from the mother
liquor to produce separated CO2 sequestering product. Separation of
the product can be achieved using any convenient approach, including a
mechanical approach, e.g., where bulk excess water is drained from the
product, e.g., either by gravity alone or with the addition of vacuum,
mechanical pressing, by filtering the product from the mother liquor to
produce a filtrate, etc. Separation of bulk water produces, in certain
embodiments, a wet, dewatered precipitate.

[0120] The resultant dewatered precipitate may then be dried, as desired,
to produce a dried product. Drying can be achieved by air drying the wet
precipitate. Where the wet precipitate is air dried, air drying may be at
room or elevated temperature. In yet another embodiment, the wet
precipitate is spray dried to dry the precipitate, where the liquid
containing the precipitate is dried by feeding it through a hot gas (such
as the gaseous waste stream from the power plant), e.g., where the liquid
feed is pumped through an atomizer into a main drying chamber and a hot
gas is passed as a co-current or counter-current to the atomizer
direction. Depending on the particular drying protocol of the system, the
drying station may include a filtration element, freeze drying structure,
spray drying structure, etc. Where desired, the dewatered precipitate
product may be washed before drying. The precipitate may be washed with
freshwater, e.g., to remove salts (such as NaC1) from the dewatered
precipitate.

[0121] In certain embodiments, the precipitate product is refined (i.e.,
processed) in some manner prior to subsequent use. Refinement may include
a variety of different protocols. In certain embodiments, the product is
subjected to mechanical refinement, e.g., grinding, in order to obtain a
product with desired physical properties, e.g., particle size, etc.

[0122] FIG. 1 provides a schematic flow diagram of a process for producing
a CO2 sequestering product according to an embodiment of the
invention. In FIG. 1, saltwater from salt water source 10 is subjected to
carbonate compound precipitation conditions at precipitation step 20. As
reviewed above, term "saltwater" is employed in its conventional sense to
refer a number of different types of aqueous fluids other than fresh
water, where the term "saltwater" includes brackish water, sea water and
brine (including man-made brines, e.g., geothermal plant wastewaters,
desalination waste waters, etc), as well as other salines having a
salinity that is greater than that of freshwater. The saltwater source
from which the carbonate compound composition of the cements of the
invention is derived may be a naturally occurring source, such as a sea,
ocean, lake, swamp, estuary, lagoon, etc., or a man-made source.

[0123] In certain embodiments, the water may be obtained from the power
plant that is also providing the gaseous waste stream. For example, in
water cooled power plants, such as seawater cooled power plants, water
that has been employed by the power plant may then be sent to the
precipitation system and employed as the water in the precipitation
reaction. In certain of these embodiments, the water may be cooled prior
to entering the precipitation reactor.

[0124] In the embodiment depicted in FIG. 1, the water from saltwater
source 10 is first charged with CO2 to produce CO2 charged
water, which CO2 is then subjected to carbonate compound
precipitation conditions. As depicted in FIG. 1, a CO2 gaseous
stream 30 is contacted with the water at precipitation step 20. The
provided gaseous stream 30 is contacted with a suitable water at
precipitation step 20 to produce a CO2 charged water. By CO2
charged water is meant water that has had CO2 gas contacted with it,
where CO2 molecules have combined with water molecules to produce,
e.g., carbonic acid, bicarbonate and carbonate ion. Charging water in
this step results in an increase in the "CO2 content" of the water,
e.g., in the form of carbonic acid, bicarbonate and carbonate ion, and a
concomitant decrease in the pCO2 of the waste stream that is
contacted with the water. The CO2 charged water is acidic, having a
pH of 6 or less, such as 5 or less and including 4 or less. In certain
embodiments, the concentration of CO2 of the gas that is used to
charge the water is 10% or higher, 25% or higher, including 50% or
higher, such as 75% or even higher. Contact protocols of interest
include, but are not limited to: direct contacting protocols, e.g.,
bubbling the gas through the volume of water, concurrent contacting
means, i.e., contact between unidirectionally flowing gaseous and liquid
phase streams, countercurrent means, i.e., contact between oppositely
flowing gaseous and liquid phase streams, and the like. Thus, contact may
be accomplished through use of infusers, bubblers, fluidic Venturi
reactor, sparger, gas filter, spray, tray, or packed column reactors, and
the like, as may be convenient.

[0125] At precipitation step 20, carbonate compounds, which may be
amorphous or crystalline, are precipitated. Precipitation conditions of
interest include those that change the physical environment of the water
to produce the desired precipitate product. For example, the temperature
of the water may be raised to an amount suitable for precipitation of the
desired carbonate compound(s) to occur. In such embodiments, the
temperature of the water may be raised to a value from 5 to 70°
C., such as from 20 to 50° C. and including from 25 to 45°
C. As such, while a given set of precipitation conditions may have a
temperature ranging from 0 to 100° C., the temperature may be
raised in certain embodiments to produce the desired precipitate. In
certain embodiments, the temperature is raised using energy generated
from low or zero carbon dioxide emission sources, e.g., solar energy
source, wind energy source, hydroelectric energy source, etc. While the
pH of the water may range from 7 to 14 during a given precipitation
process, in certain embodiments the pH is raised to alkaline levels in
order to drive the precipitation of carbonate compound as desired. In
certain of these embodiments, the pH is raised to a level which minimizes
if not eliminates CO2 gas generation production during
precipitation. In these embodiments, the pH may be raised to 10 or
higher, such as 11 or higher. Where desired, the pH of the water is
raised using any convenient approach. In certain embodiments, a pH
raising agent may be employed, where examples of such agents include
oxides, hydroxides (e.g., sodium hydroxide, potassium hydroxide,
brucite), carbonates (e.g. sodium carbonate) and the like. The amount of
pH elevating agent that is added to the saltwater source will depend on
the particular nature of the agent and the volume of saltwater being
modified, and will be sufficient to raise the pH of the salt water source
to the desired value. Alternatively, the pH of the saltwater source can
be raised to the desired level by electrolysis of the water.

[0126] CO2 charging and carbonate compound precipitation may occur in
a continuous process or at separate steps. As such, charging and
precipitation may occur in the same reactor of a system, e.g., as
illustrated in FIG. 1 at step 20, according to certain embodiments of the
invention. In yet other embodiments of the invention, these two steps may
occur in separate reactors, such that the water is first charged with
CO2 in a charging reactor and the resultant CO2 charged water
is then subjected to precipitation conditions in a separate reactor.

[0127] Following production of the carbonate precipitate from the water,
the resultant precipitated carbonate compound composition is separated
from the mother liquor to produce separated carbonate compound
precipitate product, as illustrated at step 40 of FIG. 1. Separation of
the precipitate can be achieved using any convenient approach, including
a mechanical approach, e.g., where bulk excess water is drained from the
precipitated, e.g., either by gravity alone or with the addition of
vacuum, mechanical pressing, by filtering the precipitate from the mother
liquor to produce a filtrate, etc. Separation of bulk water produces a
wet, dewatered precipitate.

[0128] The resultant dewatered precipitate is then dried to produce a
product, as illustrated at step 60 of FIG. 1. Drying can be achieved by
air drying the filtrate. Where the filtrate is air dried, air drying may
be at room or elevated temperature. In yet another embodiment, the
precipitate is spray dried to dry the precipitate, where the liquid
containing the precipitate is dried by feeding it through a hot gas (such
as the gaseous waste stream from the power plant), e.g., where the liquid
feed is pumped through an atomizer into a main drying chamber and a hot
gas is passed as a co-current or counter-current to the atomizer
direction. Depending on the particular drying protocol of the system, the
drying station may include a filtration element, freeze drying structure,
spray drying structure, etc.

[0129] Where desired, the dewatered precipitate product from the
separation reactor 40 may be washed before drying, as illustrated at
optional step 50 of FIG. 1. The precipitate may be washed with
freshwater, e.g., to remove salts (such as NaCl) from the dewatered
precipitate. Used wash water may be disposed of as convenient, e.g., by
disposing of it in a tailings pond, etc.

[0130] At step 70, the dried precipitate is refined, e.g., to provide for
desired physical characteristics, such as particle size, surface area,
etc., or to add one or more components to the precipitate, such as
admixtures, aggregate, supplementary cementitious materials, etc., to
produce a final product 80.

[0131] In certain embodiments, a system is employed to perform the above
methods.

[0132] Following production of the CO2 sequestering component, e.g.,
as described above, the CO2 sequestering is then employed to produce
a non-cementitious composition of the invention, e.g., as described
above.

Utility

[0133] Compositions of the invention find use in a variety of different
applications, as reviewed above. The subject methods and systems find use
in CO2 sequestration, particularly via sequestration in a variety of
diverse man-made products. By "sequestering CO2" is meant the
removal or segregation of CO2 from a gaseous stream, such as a
gaseous waste stream, and fixating it into a stable non-gaseous form so
that the CO2 cannot escape into the atmosphere. By "CO2
sequestration" is meant the placement of CO2 into a storage stable
form, where the CO2 is fixed at least during the useful life of the
composition. As such, sequestering of CO2 according to methods of
the invention results in prevention of CO2 gas from entering the
atmosphere and long term storage of CO2 in a manner that CO2
does not become part of the atmosphere.

[0134] While preferred embodiments of the present invention have been
shown and described herein, it will be obvious to those skilled in the
art that such embodiments are provided by way of example only. Numerous
variations, changes, and substitutions will now occur to those skilled in
the art without departing from the invention. It should be understood
that various alternatives to the embodiments of the invention described
herein may be employed in practicing the invention. It is intended that
the following claims define the scope of the invention and that methods
and structures within the scope of these claims and their equivalents be
covered thereby.